Abscisic acid(ABA),hydrogen peroxide(H_(2)O_(2)) and ascorbate(AsA)–glutathione(GSH)cycle are widely known for their participation in various stresses.However,the relationship between ABA and H_(2)O_(2) levels and th...Abscisic acid(ABA),hydrogen peroxide(H_(2)O_(2)) and ascorbate(AsA)–glutathione(GSH)cycle are widely known for their participation in various stresses.However,the relationship between ABA and H_(2)O_(2) levels and the AsA–GSH cycle under drought stress in wheat has not been studied.In this study,a hydroponic experiment was conducted in wheat seedlings subjected to 15%polyethylene glycol(PEG)6000–induced dehydration.Drought stress caused the rapid accumulation of endogenous ABA and H_(2)O_(2) and significantly decreased the number of root tips compared with the control.The application of ABA significantly increased the number of root tips,whereas the application of H_(2)O_(2) markedly reduced the number of root tips,compared with that under 15%PEG-6000.In addition,drought stress markedly increased the DHA,GSH and GSSG levels,but decreased the AsA levels,AsA/DHA and GSH/GSSG ratios compared with those in the control.The activities of the four enzymes in the AsA–GSH cycle were also markedly increased under drought stress,including glutathione reductase(GR),ascorbate peroxidase(APX),monodehydroascorbate reductase(MDHAR)and dehydroascorbate reductase(DHAR),compared with those in the control.However,the application of an ABA inhibitor significantly inhibited GR,DHAR and APX activities,whereas the application of an H_(2)O_(2) inhibitor significantly inhibited DHAR and MDHAR activities.Furthermore,the application of ABA inhibitor significantly promoted the increases of H_(2)O_(2) and the application of H_(2)O_(2) inhibitor significantly blocked the increases of ABA,compared with those under 15% PEG-6000.Taken together,the results indicated that ABA and H_(2)O_(2) probably interact under drought stress in wheat;and both of them can mediate drought stress by modulating the enzymes in AsA–GSH cycle,where ABA acts as the main regulator of GR,DHAR,and APX activities,and H_(2)O_(2) acts as the main regulator of DHAR and MDHAR activities.展开更多
Hydrogen peroxide(H_(2)O_(2))has gained widespread attention as a versatile oxidant and a mild disin-fectant.Here,an electrostatic self-assembly method is applied to couple ZnSe quantum dots(QDs)with a flower-like cov...Hydrogen peroxide(H_(2)O_(2))has gained widespread attention as a versatile oxidant and a mild disin-fectant.Here,an electrostatic self-assembly method is applied to couple ZnSe quantum dots(QDs)with a flower-like covalent organic framework(COF)to form a step-scheme(S-scheme)photocata-lyst for H_(2)O_(2)production.The as-prepared S-scheme photocatalyst exhibits a broad light absorption range with an edge at 810 nm owing to the synergistic effect between the ZnSe QDs and COF.The S-scheme charge-carrier transfer mechanism is validated by performing Fermi level calculations and in-situ X-ray photoelectron and femtosecond transient absorption spectroscopies.Photolumi-nescence,time-resolved photoluminescence,photocurrent response,electrochemical impedance spectroscopy,and electron paramagnetic resonance results show that the S-scheme heterojunction not only promotes charge carrier separation but also boosts the redox ability,resulting in enhanced photocatalytic performance.Remarkably,a 10%-ZnSe QD/COF has excellent photocatalytic H_(2)O_(2)-production activity,and the optimal S-scheme composite with ethanol as the hole scavenger yields a H_(2)O_(2)-production rate of 1895 mol g^(-1)h^(-1).This study presents an example of a high-performance organic/inorganic S-scheme photocatalyst for H_(2)O_(2)production.展开更多
The optimizing utilization of ca rbon resources has drawn wide attention all over the world,while exploiting the high-efficiency catalytic routes remains a challenge.Here,a direct methanol synthesis route is realized ...The optimizing utilization of ca rbon resources has drawn wide attention all over the world,while exploiting the high-efficiency catalytic routes remains a challenge.Here,a direct methanol synthesis route is realized from pure CO and H_(2)O over 10%Cu/t-ZrO_(2) catalyst,where the time yield of methanol is144.43 mmol mol_(Cu)^(-1)h^(-1)and the methanol selectivity in hydrocarbons is 100%,The Cu species highly dispersed in the t-ZrO_(2) support lead parts of them in the cationic state.The Cu^(+)sites contribute to the dissociation of H_(2)O,providing the H*source for methanol synthesis,while the formed Cu^(0) sites promote the absorption and transfer of H*during the reaction.Moreover,the H_(2)O is even a better H resource than H_(2) due to its better dissociation effectivity in this catalytic system.The present work offers a new approach for methanol synthesis from CO and new insight into the process of supplying H donor.展开更多
It is acknowledged that injecting CO_(2) into oil reservoirs and saline aquifers for storage is a practical and affordable method for CO_(2) sequestration.Most CO_(2) produced from industrial exhaust contains impurity...It is acknowledged that injecting CO_(2) into oil reservoirs and saline aquifers for storage is a practical and affordable method for CO_(2) sequestration.Most CO_(2) produced from industrial exhaust contains impurity gases such as H_(2)S that might impact CO_(2) sequestration due to competitive adsorption.This study makes a commendable effort to explore the adsorption behavior of CO_(2)/H_(2)S mixtures in calcite slit nanopores.Grand Canonical Monte Carlo(GCMC)simulation is employed to reveal the adsorption of CO_(2),H_(2)S as well as their binary mixtures in calcite nanopores.Results show that the increase in pressure and temperature can promote and inhibit the adsorption capacity of CO_(2) and H_(2)S in calcite nanopores,respectively.CO_(2)exhibits stronger adsorption on calcite surface than H_(2)S.Electrostatic energy plays the dominating role in the adsorption behavior.Electrostatic energy accounts for 97.11%of the CO_(2)-calcite interaction energy and 56.33%of the H_(2)S-calcite interaction energy at 10 MPa and 323.15 K.The presence of H_(2)S inhibits the CO_(2) adsorption in calcite nanopores due to competitive adsorption,and a higher mole fraction of H_(2)S leads to less CO_(2) adsorption.The quantity of CO_(2) adsorbed is lessened by approximately 33%when the mole fraction of H_(2)S reaches 0.25.CO_(2) molecules preferentially occupy the regions near the po re wall and H_(2)S molecules tend to reside at the center of nanopore even when the molar ratio of CO_(2) is low,indicating that CO_(2) has an adsorption priority on the calcite surface over H_(2)S.In addition,moisture can weaken the adsorption of both CO_(2) and H_(2)S,while CO_(2) is more affected.More interestingly,we find that pure CO_(2) is more suitable to be sequestrated in the shallower formations,i.e.,500-1500 m,whereas CO_(2)with H_(2)S impurity should be settled in the deeper reservoirs.展开更多
Steering the directional carrier migration across the interface is a central mission for efficient photocatalytic reactions.In this work,an atomic-shared heterointerface is constructed between the defect-rich ZnIn_(2)...Steering the directional carrier migration across the interface is a central mission for efficient photocatalytic reactions.In this work,an atomic-shared heterointerface is constructed between the defect-rich ZnIn_(2)S_(4)(HVs-ZIS)and CoIn_(2)S_(4)(CIS)via a defect-guided heteroepitaxial growth strategy.The strong interface coupling induces adequate carriers exchanging passageway between HVs-ZIS and CIS,enhancing the internal electric field(IEF)in the ZnIn_(2)S_(4)/CoIn_(2)S_(4)(HVs-ZIS/CIS)heterostructure.The defect structure in HVs-ZIS induces an additional defect level,improving the separation efficiency of photocarriers.Moreover,promoted by the IEF and intimate heterointerface,photogenerated electrons trapped by the defect level can migrate to the valence band of CIS,contributing to massive photogenerated electrons with intense reducibility in HVs-ZIS/CIS.Consequently,the HVs-ZIS/CIS heterostructure performs a boosted H_(2)evolution activity of 33.65 mmol g^(-1)h^(-1).This work highlights the synergistic effects of defect and strong interface coupling in regulating carrier transfer and paves a brave avenue for constructing efficient heterostructure photocatalysts.展开更多
NF_(3)is commonly used as an etching and cleaning gas in semiconductor industry,however it is a strongly greenhouse gas.Therefore,the destruction of disposal NF_(3)is an urgent task to migrate the greenhouse effect.Am...NF_(3)is commonly used as an etching and cleaning gas in semiconductor industry,however it is a strongly greenhouse gas.Therefore,the destruction of disposal NF_(3)is an urgent task to migrate the greenhouse effect.Among the technologies for NF_(3)abatement,the destructive sorption of NF_(3)over metal oxides sorbents is an effective way.Thus,the search for a highly reactive and utilized sorbent for NF_(3)destruction is in great demand.In this work,AlOOH supported on carbon-sphere(AlOOH/CS)as precursors were synthesized hydrothermally and heat-treated to prepare the Al_(2)O_(3)sorbents.The influence of AlOOH/CS hydrothermal temperatures on the reactivity of derived Al_(2)O_(3)sorbents for NF_(3)destruction was investigated,and it is shown that the Al2O3 from AlOOH/CS hydro-thermalized at 120℃is superior to others.Subsequently,the optimized Al_(2)O_(3)was covered by Mn(OH)x to prepare Mn/Al_(2)O_(3)sorbents via changing hydrothermal temperatures and Mn loadings.The results show that the Mn/Al_(2)O_(3)sorbents are more utilized than bare Al_(2)O_(3)in NF_(3)destructive sorption due to the promotional effect of Mn_(2)O_(3)as surface layer on the fluorination of Al_(2)O_(3)as substrate,especially the optimal 5%Mn/Al2O3(160℃)exhibits a utilization percentage as high as 90.4%,and remarkably exceeds all the sorbents reported so far.These findings are beneficial to develop more efficient sorbents for the destruction of NF_(3).展开更多
Hybrid nanofluids are remarkable functioning liquids that are intended to reduce the energy loss while maximizing the heat transmission.In the involvement of suction and nonlinear thermal radiation effects,this study ...Hybrid nanofluids are remarkable functioning liquids that are intended to reduce the energy loss while maximizing the heat transmission.In the involvement of suction and nonlinear thermal radiation effects,this study attempted to explore the energy transmission features of the inclined magnetohydrodynamic(MHD)stagnation flow of CNTs-hybrid nanofluid across the nonlinear permeable stretching or shrinking sheet.This work also included some noteworthy features like chemical reactions,variable molecular diffusivity,quadratic convection,viscous dissipation,velocity slip and heat omission assessment.Employing appropriate similarity components,the model equations were modified to ODEs and computed by using the HAM technique.The impact of various relevant flow characteristics on movement,heat and concentration profiles was investigated and plotted on a graph.Considering various model factors,the significance of drag friction,heat and mass transfer rate were also computed in tabular and graphical form.This leads to the conclusion that such factors have a considerable impact on the dynamics of fluid as well as other engineering measurements of interest.Furthermore,viscous forces are dominated by increasing the values ofλ_(p),δ_(m)andδ_(q),and as a result,F(ξ)accelerates while the opposite trend is observed for M andφ.The drag friction is boosted by the augmentation M,λ_(p)andφ,but the rate of heat transfer declined.According to our findings,hybrid nanoliquid effects dominate that of ordinary nanofluid in terms of F(ξ),Θ(ξ)andφ(ξ)profiles.The HAM and the numerical technique(shooting method)were found to be in good agreement.展开更多
Kathon(CMI-MI),a mixture of 5-chloro-2-methyl-4-isothiazolin-3-one(CMI)and 2-methyl-4-isothiazolin-3-one(MI),was extensively used in industry as a nonoxidizing biocide or disinfectant.However,it would show adverse eff...Kathon(CMI-MI),a mixture of 5-chloro-2-methyl-4-isothiazolin-3-one(CMI)and 2-methyl-4-isothiazolin-3-one(MI),was extensively used in industry as a nonoxidizing biocide or disinfectant.However,it would show adverse effects on aquatic life when it is discharged into surface water.In this study,the removal performance,parameter influence,degradation products and enhancement of subsequent biodegradation of CMI-MI in UV/H_(2)O_(2)system were systematically investigated.The degradation rate of CMI-MI could reach 90%under UV irradiation for 20 min when the dosage of H_(2)O_(2)was 0.3 mmol·L^(–1).The DOC(dissolved organic carbon)mineralization rate of CMI-MI could reach 35%under certain conditions([H_(2)O_(2)]=0.3 mmol·L^(–1),UV irradiation for 40 min).kobs was inversely proportional to the concentration of CMI-MI and proportional to the concentration of H_(2)O_(2).The degradation rate of CMIMI was almost unchanged in the pH range from 4 to 10.Except the presence of CO_(3)^(2-)inhibited the removal rate of CMI-MI,SO_(4)^(2-),Cl^(-),NO_(3)^(-),and NH_(4)^(+) did not interfere with the degradation of CMI-MI in the system.It was found that UV/H_(2)O_(2)system had lower energy consumption and more economic advantage compared with UV/PS system by comparing the EEO(electric energy per order)values under the same conditions.Two main organic products were identified,namely HCOOH and CH_(3)NH_(2).There’s also the formation of Cl^(-)and SO_(4)^(2-).After UV and UV/H_(2)O_(2)photolysis,the biochemical properties of CMI-MI solution were obviously improved,especially the UV/H_(2)O_(2)treatment effect was better,indicating that UV/H_(2)O_(2)technology is expected to combine with biotechnology to remove CMI-MI effectively and environmentally friendly from wastewater.展开更多
The existence and risk of emerging organic contaminants(EOCs)have been under consideration and paid much effort to degrade these pollutants.Fenton system is one of the most widely used technologies to solve this probl...The existence and risk of emerging organic contaminants(EOCs)have been under consideration and paid much effort to degrade these pollutants.Fenton system is one of the most widely used technologies to solve this problem.The original Fenton system relies on the hydroxyl radicals produced by Fe(Ⅱ)/H_(2)O_(2) to oxidize the organic contaminants.However,the application of the Fenton system is limited by its low iron cycling efficiency and the high risks of hydrogen peroxide transportation and storage.The introduction of external energy(including light and electricity etc.)can effectively promote the Fe(Ⅲ)/Fe(Ⅱ)cycle and the reduction of oxygen to produce hydrogen peroxide in situ.This review introduces three in-situ Fenton systems,which are electro-Fenton,Photo-Fenton,and chemical reaction.The mechanism,influencing factors,and catalysts of these three in-situ Fenton systems in degrading EOCs are discussed systematically.This review strengthens the understanding of Fenton and in-situ Fenton systems in degradation,offering further insight into the real application of the in-situ Fenton system in the removal of EOCs.展开更多
The deep-processing utility of pure hydrogen sulfide (H_(2)S) is a significant direction in natural gas chemical industry.Herein,a brand-new strategy of H_(2)S conversion by a,β-unsaturated carboxylate esters into th...The deep-processing utility of pure hydrogen sulfide (H_(2)S) is a significant direction in natural gas chemical industry.Herein,a brand-new strategy of H_(2)S conversion by a,β-unsaturated carboxylate esters into thiols or thioethers using task-specific carboxylate ionic liquids (ILs) as catalyst has been developed,firstly accomplishing the phase separation of product and catalyst without introducing the third component.It can be considered as a cascade reaction in which the product selectivity can be controlled by adjusting the molar ratio of H_(2)S to a,β-unsaturated carboxylate esters.Also,the effects of ILs with different anions and cations,intermittent feeding operations,as well as pressure-time kinetic behaviors on cascade reaction were investigated.Furthermore,the proposed interaction mechanism of H_(2)S conversion using butyl acrylate catalyzed by[Emim][Ac]was revealed by DFT-based theoretical calculation.The approach enables the self-phase separation promotion of catalyst and product and achieves 99%quantitative conversion under mild conditions in the absence of solvent,making the entire process ecologically benign.High-efficiency reaction activity can still be maintained after ten cycles of the catalyst.Therefore,the good results,combined with its simplicity of operation and the high recyclability of the catalyst,make this green method environmentally friendly and cost-effective.It is anticipated that this self-separation method mediated by task-specific ILs will provide a feasible strategy for H_(2)S utilization,which will guide its application on an industrial scale.展开更多
This future article discusses the new prospects and directions of CO_(2)conversion via the photo-electrocatalytic(PEC)route.The second(2nd)generation solar fuels and chemicals(SFs)are generated directly in PEC systems...This future article discusses the new prospects and directions of CO_(2)conversion via the photo-electrocatalytic(PEC)route.The second(2nd)generation solar fuels and chemicals(SFs)are generated directly in PEC systems via electrons/protons reactions without forming molecular H_(2)as an intermediate,overcoming the thermodynamics limitations and practical issues encountered for electro-fuels produced by multistep thermocatalytic processes(i.e.CO_(2)conversion with H_(2)coming from water electrolysis).A distributed and decentralized production of SFs requires very compact,highly integrated,and intensified technologies.Among the existing reactors of advanced design(based on artificial leaves or photosynthesis),the integrated photovoltaic plus electrocatalytic(PV-EC)device is the only system(demonstrated at large scale)to produce SFs with high solar-to-fuel(STF)efficiency.However,while the literature indicates STF efficiency as the main(and only)measure of process performance,we remark here the need to refer to productivity(in terms of current density)and make tests with reliable flow PEC systems(with electrodes of at least 5–10 cm^(2))to accelerate the scaling-up process.Using approaches that minimize downstream separation costs is also mandatory.Many limitations exist in PEC systems,but most can be overcome by proper electrode and cell engineering,thus going beyond the properties of the electrocatalysts.As examples of current developments,we present the progress of(i)artificial leaf/tree devices for green H_(2)distributed production and(ii)a PEC device producing the same chemicals at both cathode and anode parts without downstream operations for green solvent distributed production.Based on these developments,future directions,such as producing fertilizers and food components from the air,are outlined.The aim is to provide new ideas and research directions from a personal perspective.展开更多
The efficacy of the oxygen reduction reaction(ORR) in fuel cells can be significantly enhanced by optimizing cobalt-based catalysts,which provide a more stable alternative to iron-based catalysts.However,their perform...The efficacy of the oxygen reduction reaction(ORR) in fuel cells can be significantly enhanced by optimizing cobalt-based catalysts,which provide a more stable alternative to iron-based catalysts.However,their performance is often impeded by weak adsorption of oxygen species,leading to a 2e^(-)pathway that negatively affects fuel cell discharge efficiency.Here,we engineered a high-density cobalt active center catalyst,coordinated with nitrogen and sulfur atoms on a porous carbon substrate.Both experimental and theoretical analyses highlighted the role of sulfur atoms as electron donors,disrupting the charge symmetry of the original Co active center and promoting enhanced interaction with Co 3d orbitals.This modification improves the adsorption of oxygen and reaction intermediates during ORR,significantly reducing the production of hydrogen peroxide(H_(2)O_(2)).Remarkably,the optimized catalyst demonstrated superior fuel cell performance,with peak power densities of 1.32 W cm^(-2) in oxygen and 0.61 W cm^(-2) in air environments,respectively.A significant decrease in H_(2)O_(2) by-product accumulation was observed during the reaction process,reducing catalyst and membrane damage and consequently improving fuel cell durability.This study emphasizes the critical role of coordination symmetry in Co/N/C catalysts and proposes an effective strategy to enhance fuel cell performance.展开更多
Hydrazine oxidation reaction(HzOR)assisted hydrogen evolution reaction(HER)offers a feasible path for low power consumption to hydrogen production.Unfortunately however,the total electrooxidation of hydrazine in anode...Hydrazine oxidation reaction(HzOR)assisted hydrogen evolution reaction(HER)offers a feasible path for low power consumption to hydrogen production.Unfortunately however,the total electrooxidation of hydrazine in anode and the dissociation kinetics of water in cathode are critically depend on the interaction between the reaction intermediates and surface of catalysts,which are still challenging due to the totally different catalytic mechanisms.Herein,the[W–O]group with strong adsorption capacity is introduced into CoP nanoflakes to fabricate bifunctional catalyst,which possesses excellent catalytic performances towards both HER(185.60 mV at 1000 mA cm^(−2))and HzOR(78.99 mV at 10,00 mA cm^(−2))with the overall electrolyzer potential of 1.634 V lower than that of the water splitting system at 100 mA cm^(−2).The introduction of[W–O]groups,working as the adsorption sites for H2O dissociation and N2H4 dehydrogenation,leads to the formation of porous structure on CoP nanoflakes and regulates the electronic structure of Co through the linked O in[W–O]group as well,resultantly boosting the hydrogen production and HzOR.Moreover,a proof-of-concept direct hydrazine fuel cell-powered H_(2) production system has been assembled,realizing H_(2)evolution at a rate of 3.53 mmol cm^(−2)h^(−1)at room temperature without external electricity supply.展开更多
The challenge of high temperatures in deep mining remains harmful to the health of workers and their production efficiency The addition of phase change materials (PCMs) to filling slurry and the use of the cold storag...The challenge of high temperatures in deep mining remains harmful to the health of workers and their production efficiency The addition of phase change materials (PCMs) to filling slurry and the use of the cold storage function of these materials to reduce downhole temperatures is an effective approach to alleviate the aforementioned problem.Paraffin–CaCl_(2)·6H_(2)O composite PCM was prepared in the laboratory.The composition,phase change latent heat,thermal conductivity,and cemented tailing backfill (CTB) compressive strength of the new material were studied.The heat transfer characteristics and endothermic effect of the PCM were simulated using Fluent software.The results showed the following:(1) The new paraffin–CaCl_(2)·6H_(2)O composite PCM improved the thermal conductivity of native paraffin while avoiding the water solubility of CaCl_(2)·6H_(2)O.(2) The calculation formula of the thermal conductivity of CaCl_(2)·6H_(2)O combined with paraffin was deduced,and the reasons were explained in principle.(3) The“enthalpy–mass scale model”was applied to calculate the phase change latent heat of nonreactive composite PCMs.(4)The addition of the paraffin–CaCl_(2)·6H_(2)O composite PCM reduced the CTB strength but increased its heat absorption capacity.This research can give a theoretical foundation for the use of heat storage backfill in green mines.展开更多
V_(3)O_(7)·H_(2)O(VO)is a high capacity cathode material in the field of aqueous zinc ion batteries(AZIBs),but it is limited by slow ion migration and low electrical conductivity.In this paper,polypyridine(PPyd)i...V_(3)O_(7)·H_(2)O(VO)is a high capacity cathode material in the field of aqueous zinc ion batteries(AZIBs),but it is limited by slow ion migration and low electrical conductivity.In this paper,polypyridine(PPyd)intercalated VO with nanoribbon structure was prepared by a simple in-situ pre-intercalation,which is noted VO-PPyd.The total density of states(TDOS)shows that after the pre-intercalation of PPyd,an intermediate energy level appears between the valence band and conduction band,which provides a step that can effectively reduce the band gap and enhance the electron conductivity.Furthermore,the density functional theory(DFT)results found that Zn^(2+)is more easily de-intercalated from the V-O skeleton,which proves that the embeddedness of PPyd improves the diffusion kinetics of Zn^(2+).Electrochemical studies have shown that VO-PPyd cathode materials exhibit excellent rate performance(high specific capacity of 465 and 192 mA h g^(-1)at 0.2 and 10 A g^(-1),respectively)and long-term cycling performance(92.7%capacity retention rate after 5300 cycles),due to their advantages in structure and composition.More importantly,the energy density of VO-PPyd//Zn at 581 and 5806 W kg^(-1)is 375 and 247 W h kg^(-1),respectively.VO-PPyd exhibits excellent electrochemical properties compared to previously reported vanadium based cathodes,which makes it highly competitive in the field of high-performance cathode materials of AZIBs.展开更多
In spite of the numerous advances in the development of H_(2)and O_(2)evolutions upon water splitting,the separation of H_(2)from O_(2)still remains a severe challenge.Herein,the novel dual-functional nanocatalysts Pd...In spite of the numerous advances in the development of H_(2)and O_(2)evolutions upon water splitting,the separation of H_(2)from O_(2)still remains a severe challenge.Herein,the novel dual-functional nanocatalysts Pd/carbon nanosphere(CNS),obtained via immobilization of ultrafine Pd nanoparticles onto CNS,are developed and employed for both selective H_(2)generation from HCOOH dehydrogenation and O_(2)evolution from H_(2)O_(2)decomposition.In these reactions,the highest activities for Pd/CNS-800(i.e.,calcinated at 800℃)are 2478 h−1 and 993 min^(−1)for H_(2)and O_(2)evolution,respectively.The highly efficient and selective“on-off”switch for selective H_(2)generation from HCOOH is successfully realized by pH adjustment.This novel and highly efficient nanocatalyst Pd/CNS-800 not only provides new approaches for the promising application of HCOOH and H_(2)O_(2)as economic and safe H_(2)and O_(2)carriers,respectively,for fuel cells,but also promotes the development of“on-off”switch for on-demand H_(2)evolution.展开更多
Utilizing the hydrazine-assisted water electrolysis for energy-efficient hydrogen production shows a promising application, which relies on the development and design of efficient bifunctional electrocatalysts. Herein...Utilizing the hydrazine-assisted water electrolysis for energy-efficient hydrogen production shows a promising application, which relies on the development and design of efficient bifunctional electrocatalysts. Herein, we reported a low-content Pt-doped Rh metallene(Pt-Rhene) for hydrazine-assisted water electrolysis towards energy-saving hydrogen(H_(2)) production, where the ultrathin metallene is constructed to provide enough favorable active sites for catalysis and improve atom utilization.Additionally, the synergistic effect between Rh and Pt can optimize the electronic structure of Rh for improving the intrinsic activity. Therefore, the required overpotential of Pt-Rhene is only 37 mV to reach a current density of-10 mA cm^(-2) in the hydrogen evolution reaction(HER), and the Pt-Rhene exhibits a required overpotential of only 11 mV to reach a current density of 10 mA cm^(-2) in the hydrazine oxidation reaction(HzOR). With the constructed HER-HzOR two-electrode system, the Pt-Rhene electrodes exhibit an extremely low voltage(0.06/0.19/0.28 V) to achieve current densities of 10/50/100 mA cm^(-2) for energy-saving H_(2) production, which greatly reduces the electrolysis energy consumption. Moreover,DFT calculations further demonstrate that the introduction of Pt modulates the electronic structure of Rh and optimizes the d-band center, thus enhancing the adsorption and desorption of reactant/intermediates in the electrocatalytic reaction.展开更多
With the application of resins in various fields, numerous waste resins that are difficult to treat have been produced. The industrial wastewater containing Cr(Ⅵ) has severely polluted soil and groundwater environmen...With the application of resins in various fields, numerous waste resins that are difficult to treat have been produced. The industrial wastewater containing Cr(Ⅵ) has severely polluted soil and groundwater environments, thereby endangering human health. Therefore, in this paper, a novel functionalized mesoporous adsorbent PPR-Z was synthesized from waste amidoxime resin for adsorbing Cr(Ⅵ). The waste amidoxime resin was first modified with H3PO4 and ZnCl_(2), and subsequently, it was carbonized through slow thermal decomposition. The static adsorption of PPR-Z conforms to the pseudo-second-order kinetic model and Langmuir isotherm, indicating that the Cr(Ⅵ) adsorption by PPR-Z is mostly chemical adsorption and exhibits single-layer adsorption. The saturated adsorption capacity of the adsorbent for Cr(Ⅵ) could reach 255.86 mg/g. The adsorbent could effectively reduce Cr(Ⅵ) to Cr(Ⅲ) and decrease the toxicity of Cr(Ⅵ) during adsorption. PPR-Z exhibited Cr(Ⅵ) selectivity in electroplating wastewater. The main mechanisms involved in the Cr(Ⅵ) adsorption are the chemical reduction of Cr(Ⅵ) into Cr(Ⅲ) and electrostatic and coordination interactions. Preparation of PPR-Z not only solves the problem of waste resin treatment but also effectively controls Cr(Ⅵ) pollution and realizes the concept of “treating waste with waste”.展开更多
Numerous decision-makers in politics,science,and business worldwide have acknowledged that hydrogen H_(2) will become one of the most important energy sources of the 21st century if the desired energy transition to ca...Numerous decision-makers in politics,science,and business worldwide have acknowledged that hydrogen H_(2) will become one of the most important energy sources of the 21st century if the desired energy transition to carbon-free energy sources is to be taken seriously.Nevertheless,this transition in general and the introduction of H_(2) in particular is still progressing far too slowly.There are now countless projects worldwide,including several worth billions of US dollars,but we are still waiting for the breakthrough.There seem to be various reasons for this,not just one single or most important one.Purpose:In the overall context of global earth overheating(often downplayed as“climate change”),hydrogen H_(2) will undoubtedly play a decisive role as of now.The paper aims to identify the key challenges and propose solutions for establishing a sustainable value chain for market penetration of H_(2).Design/methodology/approach:This paper aims to shed light on the current situation using freely accessible publications from global management consultancies and the German government,as well as critical reporting.The problem of human behavior is also explained by the Novak Triangle.Findings:Most people have come to understand that anthropogenic global overheating can only be solved by new technologies(which cost money,time,and behavioral change)in production and application.Hydrogen H_(2) appears to be an essential part of the desired solution.Nevertheless,there are currently still numerous challenges and also concrete concerns worldwide,which partially cast the implementation in a questionable light.The findings suggest that establishing a demand and supply of H_(2) needs a comprehensive infrastructure,circular economy principles,and changes in consumer behavior and policy frameworks.The paper proposes solutions for addressing these challenges.Affected countries:The situation described here relates to Germany and the EU countries,but it is likely to be comparable,or at least similar,for many industrialized countries.The challenges and solutions proposed in this paper are relevant to countries worldwide that are transitioning to sustainable energy and transportation systems.Research/future/practical implications:As of 2024,it must be stated that the implementation of H_(2) is still progressing far too slowly,even in the“model country”Germany.There are still problems and stalling in many places.The biggest challenge seems to be the problem:without demand,there is no supply;without supply,there is no demand.This can then best be achieved with simple“out-of-the-box”solutions in mindset(see Novak triangle).The research implications of this paper include the need for further research on the challenges of establishing a sustainable value chain and the effectiveness of the proposed solutions.The future implications of this paper include the importance of establishing a sustainable value chain to mitigate climate change and reduce dependence on fossil fuels.The core point will become the collaboration across the entire value chain to establish a sustainable infrastructure for sustainable energy and transportation systems.Originality/value:Currently,there are virtually no scientific books that would present the overall context of the challenges.Therefore,only current surveys,market volumes,and challenges in environmental and working conditions can be described here.This paper contributes to the literature by analyzing the challenges of establishing a market model for hydrogen H_(2).The paper proposes solutions for addressing these challenges and shows difficulties.It provides valuable insights for policymakers,industry stakeholders,and researchers working towards a sustainable energy future.展开更多
基金This research was funded by the National Key Research and Development Program of China(2023YFD2301505).
文摘Abscisic acid(ABA),hydrogen peroxide(H_(2)O_(2)) and ascorbate(AsA)–glutathione(GSH)cycle are widely known for their participation in various stresses.However,the relationship between ABA and H_(2)O_(2) levels and the AsA–GSH cycle under drought stress in wheat has not been studied.In this study,a hydroponic experiment was conducted in wheat seedlings subjected to 15%polyethylene glycol(PEG)6000–induced dehydration.Drought stress caused the rapid accumulation of endogenous ABA and H_(2)O_(2) and significantly decreased the number of root tips compared with the control.The application of ABA significantly increased the number of root tips,whereas the application of H_(2)O_(2) markedly reduced the number of root tips,compared with that under 15%PEG-6000.In addition,drought stress markedly increased the DHA,GSH and GSSG levels,but decreased the AsA levels,AsA/DHA and GSH/GSSG ratios compared with those in the control.The activities of the four enzymes in the AsA–GSH cycle were also markedly increased under drought stress,including glutathione reductase(GR),ascorbate peroxidase(APX),monodehydroascorbate reductase(MDHAR)and dehydroascorbate reductase(DHAR),compared with those in the control.However,the application of an ABA inhibitor significantly inhibited GR,DHAR and APX activities,whereas the application of an H_(2)O_(2) inhibitor significantly inhibited DHAR and MDHAR activities.Furthermore,the application of ABA inhibitor significantly promoted the increases of H_(2)O_(2) and the application of H_(2)O_(2) inhibitor significantly blocked the increases of ABA,compared with those under 15% PEG-6000.Taken together,the results indicated that ABA and H_(2)O_(2) probably interact under drought stress in wheat;and both of them can mediate drought stress by modulating the enzymes in AsA–GSH cycle,where ABA acts as the main regulator of GR,DHAR,and APX activities,and H_(2)O_(2) acts as the main regulator of DHAR and MDHAR activities.
文摘Hydrogen peroxide(H_(2)O_(2))has gained widespread attention as a versatile oxidant and a mild disin-fectant.Here,an electrostatic self-assembly method is applied to couple ZnSe quantum dots(QDs)with a flower-like covalent organic framework(COF)to form a step-scheme(S-scheme)photocata-lyst for H_(2)O_(2)production.The as-prepared S-scheme photocatalyst exhibits a broad light absorption range with an edge at 810 nm owing to the synergistic effect between the ZnSe QDs and COF.The S-scheme charge-carrier transfer mechanism is validated by performing Fermi level calculations and in-situ X-ray photoelectron and femtosecond transient absorption spectroscopies.Photolumi-nescence,time-resolved photoluminescence,photocurrent response,electrochemical impedance spectroscopy,and electron paramagnetic resonance results show that the S-scheme heterojunction not only promotes charge carrier separation but also boosts the redox ability,resulting in enhanced photocatalytic performance.Remarkably,a 10%-ZnSe QD/COF has excellent photocatalytic H_(2)O_(2)-production activity,and the optimal S-scheme composite with ethanol as the hole scavenger yields a H_(2)O_(2)-production rate of 1895 mol g^(-1)h^(-1).This study presents an example of a high-performance organic/inorganic S-scheme photocatalyst for H_(2)O_(2)production.
基金supported by the National Natural Science Foundation of China under grant numbers 22172032,U22A20431 and U19B2003。
文摘The optimizing utilization of ca rbon resources has drawn wide attention all over the world,while exploiting the high-efficiency catalytic routes remains a challenge.Here,a direct methanol synthesis route is realized from pure CO and H_(2)O over 10%Cu/t-ZrO_(2) catalyst,where the time yield of methanol is144.43 mmol mol_(Cu)^(-1)h^(-1)and the methanol selectivity in hydrocarbons is 100%,The Cu species highly dispersed in the t-ZrO_(2) support lead parts of them in the cationic state.The Cu^(+)sites contribute to the dissociation of H_(2)O,providing the H*source for methanol synthesis,while the formed Cu^(0) sites promote the absorption and transfer of H*during the reaction.Moreover,the H_(2)O is even a better H resource than H_(2) due to its better dissociation effectivity in this catalytic system.The present work offers a new approach for methanol synthesis from CO and new insight into the process of supplying H donor.
基金financial support from the National Natural Science Foundation of China (Grant No.52004320)the Science Foundation of China University of Petroleum,Beijing (No.2462021QNXZ012,No.2462022BJRC001,and No.2462021YJRC012)the funding from the State Key Laboratory of Petroleum Resources and Engineering (No.PRP/indep-1-2103)。
文摘It is acknowledged that injecting CO_(2) into oil reservoirs and saline aquifers for storage is a practical and affordable method for CO_(2) sequestration.Most CO_(2) produced from industrial exhaust contains impurity gases such as H_(2)S that might impact CO_(2) sequestration due to competitive adsorption.This study makes a commendable effort to explore the adsorption behavior of CO_(2)/H_(2)S mixtures in calcite slit nanopores.Grand Canonical Monte Carlo(GCMC)simulation is employed to reveal the adsorption of CO_(2),H_(2)S as well as their binary mixtures in calcite nanopores.Results show that the increase in pressure and temperature can promote and inhibit the adsorption capacity of CO_(2) and H_(2)S in calcite nanopores,respectively.CO_(2)exhibits stronger adsorption on calcite surface than H_(2)S.Electrostatic energy plays the dominating role in the adsorption behavior.Electrostatic energy accounts for 97.11%of the CO_(2)-calcite interaction energy and 56.33%of the H_(2)S-calcite interaction energy at 10 MPa and 323.15 K.The presence of H_(2)S inhibits the CO_(2) adsorption in calcite nanopores due to competitive adsorption,and a higher mole fraction of H_(2)S leads to less CO_(2) adsorption.The quantity of CO_(2) adsorbed is lessened by approximately 33%when the mole fraction of H_(2)S reaches 0.25.CO_(2) molecules preferentially occupy the regions near the po re wall and H_(2)S molecules tend to reside at the center of nanopore even when the molar ratio of CO_(2) is low,indicating that CO_(2) has an adsorption priority on the calcite surface over H_(2)S.In addition,moisture can weaken the adsorption of both CO_(2) and H_(2)S,while CO_(2) is more affected.More interestingly,we find that pure CO_(2) is more suitable to be sequestrated in the shallower formations,i.e.,500-1500 m,whereas CO_(2)with H_(2)S impurity should be settled in the deeper reservoirs.
基金supported by the National Natural Science Foundation of China(52072196,52002200,52102106,52202262,22379081,22379080)the Major Basic Research Program of Natural Science Foundation of Shandong Province(ZR2020ZD09)+1 种基金the Natural Science Foundation of Shandong Province(ZR2020QE063,ZR202108180009,ZR2023QE059)the Project funded by China Postdoctoral Science Foundation(2023M741871)。
文摘Steering the directional carrier migration across the interface is a central mission for efficient photocatalytic reactions.In this work,an atomic-shared heterointerface is constructed between the defect-rich ZnIn_(2)S_(4)(HVs-ZIS)and CoIn_(2)S_(4)(CIS)via a defect-guided heteroepitaxial growth strategy.The strong interface coupling induces adequate carriers exchanging passageway between HVs-ZIS and CIS,enhancing the internal electric field(IEF)in the ZnIn_(2)S_(4)/CoIn_(2)S_(4)(HVs-ZIS/CIS)heterostructure.The defect structure in HVs-ZIS induces an additional defect level,improving the separation efficiency of photocarriers.Moreover,promoted by the IEF and intimate heterointerface,photogenerated electrons trapped by the defect level can migrate to the valence band of CIS,contributing to massive photogenerated electrons with intense reducibility in HVs-ZIS/CIS.Consequently,the HVs-ZIS/CIS heterostructure performs a boosted H_(2)evolution activity of 33.65 mmol g^(-1)h^(-1).This work highlights the synergistic effects of defect and strong interface coupling in regulating carrier transfer and paves a brave avenue for constructing efficient heterostructure photocatalysts.
基金The financial support from the Natural Science Foundation of Shandong Province (ZR2020KB003)
文摘NF_(3)is commonly used as an etching and cleaning gas in semiconductor industry,however it is a strongly greenhouse gas.Therefore,the destruction of disposal NF_(3)is an urgent task to migrate the greenhouse effect.Among the technologies for NF_(3)abatement,the destructive sorption of NF_(3)over metal oxides sorbents is an effective way.Thus,the search for a highly reactive and utilized sorbent for NF_(3)destruction is in great demand.In this work,AlOOH supported on carbon-sphere(AlOOH/CS)as precursors were synthesized hydrothermally and heat-treated to prepare the Al_(2)O_(3)sorbents.The influence of AlOOH/CS hydrothermal temperatures on the reactivity of derived Al_(2)O_(3)sorbents for NF_(3)destruction was investigated,and it is shown that the Al2O3 from AlOOH/CS hydro-thermalized at 120℃is superior to others.Subsequently,the optimized Al_(2)O_(3)was covered by Mn(OH)x to prepare Mn/Al_(2)O_(3)sorbents via changing hydrothermal temperatures and Mn loadings.The results show that the Mn/Al_(2)O_(3)sorbents are more utilized than bare Al_(2)O_(3)in NF_(3)destructive sorption due to the promotional effect of Mn_(2)O_(3)as surface layer on the fluorination of Al_(2)O_(3)as substrate,especially the optimal 5%Mn/Al2O3(160℃)exhibits a utilization percentage as high as 90.4%,and remarkably exceeds all the sorbents reported so far.These findings are beneficial to develop more efficient sorbents for the destruction of NF_(3).
基金funded by King Mongkut’s University of Technology North Bangkok with Contract no.KMUTNB-Post-65-07。
文摘Hybrid nanofluids are remarkable functioning liquids that are intended to reduce the energy loss while maximizing the heat transmission.In the involvement of suction and nonlinear thermal radiation effects,this study attempted to explore the energy transmission features of the inclined magnetohydrodynamic(MHD)stagnation flow of CNTs-hybrid nanofluid across the nonlinear permeable stretching or shrinking sheet.This work also included some noteworthy features like chemical reactions,variable molecular diffusivity,quadratic convection,viscous dissipation,velocity slip and heat omission assessment.Employing appropriate similarity components,the model equations were modified to ODEs and computed by using the HAM technique.The impact of various relevant flow characteristics on movement,heat and concentration profiles was investigated and plotted on a graph.Considering various model factors,the significance of drag friction,heat and mass transfer rate were also computed in tabular and graphical form.This leads to the conclusion that such factors have a considerable impact on the dynamics of fluid as well as other engineering measurements of interest.Furthermore,viscous forces are dominated by increasing the values ofλ_(p),δ_(m)andδ_(q),and as a result,F(ξ)accelerates while the opposite trend is observed for M andφ.The drag friction is boosted by the augmentation M,λ_(p)andφ,but the rate of heat transfer declined.According to our findings,hybrid nanoliquid effects dominate that of ordinary nanofluid in terms of F(ξ),Θ(ξ)andφ(ξ)profiles.The HAM and the numerical technique(shooting method)were found to be in good agreement.
基金support of experimental Instrument Platform of Shandong Taihe Water Treatment Technology Co.,LTD.
文摘Kathon(CMI-MI),a mixture of 5-chloro-2-methyl-4-isothiazolin-3-one(CMI)and 2-methyl-4-isothiazolin-3-one(MI),was extensively used in industry as a nonoxidizing biocide or disinfectant.However,it would show adverse effects on aquatic life when it is discharged into surface water.In this study,the removal performance,parameter influence,degradation products and enhancement of subsequent biodegradation of CMI-MI in UV/H_(2)O_(2)system were systematically investigated.The degradation rate of CMI-MI could reach 90%under UV irradiation for 20 min when the dosage of H_(2)O_(2)was 0.3 mmol·L^(–1).The DOC(dissolved organic carbon)mineralization rate of CMI-MI could reach 35%under certain conditions([H_(2)O_(2)]=0.3 mmol·L^(–1),UV irradiation for 40 min).kobs was inversely proportional to the concentration of CMI-MI and proportional to the concentration of H_(2)O_(2).The degradation rate of CMIMI was almost unchanged in the pH range from 4 to 10.Except the presence of CO_(3)^(2-)inhibited the removal rate of CMI-MI,SO_(4)^(2-),Cl^(-),NO_(3)^(-),and NH_(4)^(+) did not interfere with the degradation of CMI-MI in the system.It was found that UV/H_(2)O_(2)system had lower energy consumption and more economic advantage compared with UV/PS system by comparing the EEO(electric energy per order)values under the same conditions.Two main organic products were identified,namely HCOOH and CH_(3)NH_(2).There’s also the formation of Cl^(-)and SO_(4)^(2-).After UV and UV/H_(2)O_(2)photolysis,the biochemical properties of CMI-MI solution were obviously improved,especially the UV/H_(2)O_(2)treatment effect was better,indicating that UV/H_(2)O_(2)technology is expected to combine with biotechnology to remove CMI-MI effectively and environmentally friendly from wastewater.
基金supported by the National Natural Science Foundation of China(No.21906056No.22176060)+2 种基金the Undergraduate Training Program on Innovation and Entrepreneurship(S202110251087)the Science and Technology Commission of Shanghai Municipality(22ZR1418600)Shanghai Municipal Science and Technology(No.20DZ2250400).
文摘The existence and risk of emerging organic contaminants(EOCs)have been under consideration and paid much effort to degrade these pollutants.Fenton system is one of the most widely used technologies to solve this problem.The original Fenton system relies on the hydroxyl radicals produced by Fe(Ⅱ)/H_(2)O_(2) to oxidize the organic contaminants.However,the application of the Fenton system is limited by its low iron cycling efficiency and the high risks of hydrogen peroxide transportation and storage.The introduction of external energy(including light and electricity etc.)can effectively promote the Fe(Ⅲ)/Fe(Ⅱ)cycle and the reduction of oxygen to produce hydrogen peroxide in situ.This review introduces three in-situ Fenton systems,which are electro-Fenton,Photo-Fenton,and chemical reaction.The mechanism,influencing factors,and catalysts of these three in-situ Fenton systems in degrading EOCs are discussed systematically.This review strengthens the understanding of Fenton and in-situ Fenton systems in degradation,offering further insight into the real application of the in-situ Fenton system in the removal of EOCs.
基金sponsored by the National Natural Science Foundation of China (Nos. 22208140 and 22078145)。
文摘The deep-processing utility of pure hydrogen sulfide (H_(2)S) is a significant direction in natural gas chemical industry.Herein,a brand-new strategy of H_(2)S conversion by a,β-unsaturated carboxylate esters into thiols or thioethers using task-specific carboxylate ionic liquids (ILs) as catalyst has been developed,firstly accomplishing the phase separation of product and catalyst without introducing the third component.It can be considered as a cascade reaction in which the product selectivity can be controlled by adjusting the molar ratio of H_(2)S to a,β-unsaturated carboxylate esters.Also,the effects of ILs with different anions and cations,intermittent feeding operations,as well as pressure-time kinetic behaviors on cascade reaction were investigated.Furthermore,the proposed interaction mechanism of H_(2)S conversion using butyl acrylate catalyzed by[Emim][Ac]was revealed by DFT-based theoretical calculation.The approach enables the self-phase separation promotion of catalyst and product and achieves 99%quantitative conversion under mild conditions in the absence of solvent,making the entire process ecologically benign.High-efficiency reaction activity can still be maintained after ten cycles of the catalyst.Therefore,the good results,combined with its simplicity of operation and the high recyclability of the catalyst,make this green method environmentally friendly and cost-effective.It is anticipated that this self-separation method mediated by task-specific ILs will provide a feasible strategy for H_(2)S utilization,which will guide its application on an industrial scale.
基金the EU for providing support to these activities through the EU projects DECADE(862030),EPOCH(101070976)and SCOPE(810182)。
文摘This future article discusses the new prospects and directions of CO_(2)conversion via the photo-electrocatalytic(PEC)route.The second(2nd)generation solar fuels and chemicals(SFs)are generated directly in PEC systems via electrons/protons reactions without forming molecular H_(2)as an intermediate,overcoming the thermodynamics limitations and practical issues encountered for electro-fuels produced by multistep thermocatalytic processes(i.e.CO_(2)conversion with H_(2)coming from water electrolysis).A distributed and decentralized production of SFs requires very compact,highly integrated,and intensified technologies.Among the existing reactors of advanced design(based on artificial leaves or photosynthesis),the integrated photovoltaic plus electrocatalytic(PV-EC)device is the only system(demonstrated at large scale)to produce SFs with high solar-to-fuel(STF)efficiency.However,while the literature indicates STF efficiency as the main(and only)measure of process performance,we remark here the need to refer to productivity(in terms of current density)and make tests with reliable flow PEC systems(with electrodes of at least 5–10 cm^(2))to accelerate the scaling-up process.Using approaches that minimize downstream separation costs is also mandatory.Many limitations exist in PEC systems,but most can be overcome by proper electrode and cell engineering,thus going beyond the properties of the electrocatalysts.As examples of current developments,we present the progress of(i)artificial leaf/tree devices for green H_(2)distributed production and(ii)a PEC device producing the same chemicals at both cathode and anode parts without downstream operations for green solvent distributed production.Based on these developments,future directions,such as producing fertilizers and food components from the air,are outlined.The aim is to provide new ideas and research directions from a personal perspective.
基金financially National Natural Science Foundation of China (22288102, 22172134, U1932201, U2032202)Science and Technology Planning Project of Fujian Province (2022H0002)support from the EPSRC (EP/W03784X/1)。
文摘The efficacy of the oxygen reduction reaction(ORR) in fuel cells can be significantly enhanced by optimizing cobalt-based catalysts,which provide a more stable alternative to iron-based catalysts.However,their performance is often impeded by weak adsorption of oxygen species,leading to a 2e^(-)pathway that negatively affects fuel cell discharge efficiency.Here,we engineered a high-density cobalt active center catalyst,coordinated with nitrogen and sulfur atoms on a porous carbon substrate.Both experimental and theoretical analyses highlighted the role of sulfur atoms as electron donors,disrupting the charge symmetry of the original Co active center and promoting enhanced interaction with Co 3d orbitals.This modification improves the adsorption of oxygen and reaction intermediates during ORR,significantly reducing the production of hydrogen peroxide(H_(2)O_(2)).Remarkably,the optimized catalyst demonstrated superior fuel cell performance,with peak power densities of 1.32 W cm^(-2) in oxygen and 0.61 W cm^(-2) in air environments,respectively.A significant decrease in H_(2)O_(2) by-product accumulation was observed during the reaction process,reducing catalyst and membrane damage and consequently improving fuel cell durability.This study emphasizes the critical role of coordination symmetry in Co/N/C catalysts and proposes an effective strategy to enhance fuel cell performance.
基金support of this research by National Natural Science Foundation of China(52172110)Key Research Program of Frontier Sciences,Chinese Academy of Sciences(ZDBS-LY-SLH029)+1 种基金the“Scientific and Technical Innovation Action Plan”Hong Kong,Macao and Taiwan Science&Technology Cooperation Project of Shanghai Science and Technology Committee(21520760500)BL14W1 beamline of Shanghai Synchrotron Radiation Facility(SSRF).
文摘Hydrazine oxidation reaction(HzOR)assisted hydrogen evolution reaction(HER)offers a feasible path for low power consumption to hydrogen production.Unfortunately however,the total electrooxidation of hydrazine in anode and the dissociation kinetics of water in cathode are critically depend on the interaction between the reaction intermediates and surface of catalysts,which are still challenging due to the totally different catalytic mechanisms.Herein,the[W–O]group with strong adsorption capacity is introduced into CoP nanoflakes to fabricate bifunctional catalyst,which possesses excellent catalytic performances towards both HER(185.60 mV at 1000 mA cm^(−2))and HzOR(78.99 mV at 10,00 mA cm^(−2))with the overall electrolyzer potential of 1.634 V lower than that of the water splitting system at 100 mA cm^(−2).The introduction of[W–O]groups,working as the adsorption sites for H2O dissociation and N2H4 dehydrogenation,leads to the formation of porous structure on CoP nanoflakes and regulates the electronic structure of Co through the linked O in[W–O]group as well,resultantly boosting the hydrogen production and HzOR.Moreover,a proof-of-concept direct hydrazine fuel cell-powered H_(2) production system has been assembled,realizing H_(2)evolution at a rate of 3.53 mmol cm^(−2)h^(−1)at room temperature without external electricity supply.
基金financial support provided by the National Natural Science Foundation of China (No. 52174106)the Key Technology Research and Development Program (No. 2022YFC2905102)。
文摘The challenge of high temperatures in deep mining remains harmful to the health of workers and their production efficiency The addition of phase change materials (PCMs) to filling slurry and the use of the cold storage function of these materials to reduce downhole temperatures is an effective approach to alleviate the aforementioned problem.Paraffin–CaCl_(2)·6H_(2)O composite PCM was prepared in the laboratory.The composition,phase change latent heat,thermal conductivity,and cemented tailing backfill (CTB) compressive strength of the new material were studied.The heat transfer characteristics and endothermic effect of the PCM were simulated using Fluent software.The results showed the following:(1) The new paraffin–CaCl_(2)·6H_(2)O composite PCM improved the thermal conductivity of native paraffin while avoiding the water solubility of CaCl_(2)·6H_(2)O.(2) The calculation formula of the thermal conductivity of CaCl_(2)·6H_(2)O combined with paraffin was deduced,and the reasons were explained in principle.(3) The“enthalpy–mass scale model”was applied to calculate the phase change latent heat of nonreactive composite PCMs.(4)The addition of the paraffin–CaCl_(2)·6H_(2)O composite PCM reduced the CTB strength but increased its heat absorption capacity.This research can give a theoretical foundation for the use of heat storage backfill in green mines.
基金supported by the National Natural Science Foundation of China (21676036)the Natural Science Foundation of Chongqing (CSTB2023NSCQ-MSX0580)the Graduate Research and Innovation Foundation of Chongqing (CYB22043 and CYS22073)。
文摘V_(3)O_(7)·H_(2)O(VO)is a high capacity cathode material in the field of aqueous zinc ion batteries(AZIBs),but it is limited by slow ion migration and low electrical conductivity.In this paper,polypyridine(PPyd)intercalated VO with nanoribbon structure was prepared by a simple in-situ pre-intercalation,which is noted VO-PPyd.The total density of states(TDOS)shows that after the pre-intercalation of PPyd,an intermediate energy level appears between the valence band and conduction band,which provides a step that can effectively reduce the band gap and enhance the electron conductivity.Furthermore,the density functional theory(DFT)results found that Zn^(2+)is more easily de-intercalated from the V-O skeleton,which proves that the embeddedness of PPyd improves the diffusion kinetics of Zn^(2+).Electrochemical studies have shown that VO-PPyd cathode materials exhibit excellent rate performance(high specific capacity of 465 and 192 mA h g^(-1)at 0.2 and 10 A g^(-1),respectively)and long-term cycling performance(92.7%capacity retention rate after 5300 cycles),due to their advantages in structure and composition.More importantly,the energy density of VO-PPyd//Zn at 581 and 5806 W kg^(-1)is 375 and 247 W h kg^(-1),respectively.VO-PPyd exhibits excellent electrochemical properties compared to previously reported vanadium based cathodes,which makes it highly competitive in the field of high-performance cathode materials of AZIBs.
基金National Natural Science Foundation of China,Grant/Award Number:21805166111 Project of China,Grant/Award Number:D20015+1 种基金Ministryof Education,Hubei province,China,Grant/Award Number:T2020004Foundation of Science and Technology Bureau of Yichang City,Grant/Award Number:A21‐3‐012。
文摘In spite of the numerous advances in the development of H_(2)and O_(2)evolutions upon water splitting,the separation of H_(2)from O_(2)still remains a severe challenge.Herein,the novel dual-functional nanocatalysts Pd/carbon nanosphere(CNS),obtained via immobilization of ultrafine Pd nanoparticles onto CNS,are developed and employed for both selective H_(2)generation from HCOOH dehydrogenation and O_(2)evolution from H_(2)O_(2)decomposition.In these reactions,the highest activities for Pd/CNS-800(i.e.,calcinated at 800℃)are 2478 h−1 and 993 min^(−1)for H_(2)and O_(2)evolution,respectively.The highly efficient and selective“on-off”switch for selective H_(2)generation from HCOOH is successfully realized by pH adjustment.This novel and highly efficient nanocatalyst Pd/CNS-800 not only provides new approaches for the promising application of HCOOH and H_(2)O_(2)as economic and safe H_(2)and O_(2)carriers,respectively,for fuel cells,but also promotes the development of“on-off”switch for on-demand H_(2)evolution.
基金financially supported by the National Natural Science Foundation of China (No. 21972126, 21978264, 21905250, and 22278369)the Natural Science Foundation of Zhejiang Province (No. LQ22B030012 and LQ23B030010)the China Postdoctoral Science Foundation (2021M702889)。
文摘Utilizing the hydrazine-assisted water electrolysis for energy-efficient hydrogen production shows a promising application, which relies on the development and design of efficient bifunctional electrocatalysts. Herein, we reported a low-content Pt-doped Rh metallene(Pt-Rhene) for hydrazine-assisted water electrolysis towards energy-saving hydrogen(H_(2)) production, where the ultrathin metallene is constructed to provide enough favorable active sites for catalysis and improve atom utilization.Additionally, the synergistic effect between Rh and Pt can optimize the electronic structure of Rh for improving the intrinsic activity. Therefore, the required overpotential of Pt-Rhene is only 37 mV to reach a current density of-10 mA cm^(-2) in the hydrogen evolution reaction(HER), and the Pt-Rhene exhibits a required overpotential of only 11 mV to reach a current density of 10 mA cm^(-2) in the hydrazine oxidation reaction(HzOR). With the constructed HER-HzOR two-electrode system, the Pt-Rhene electrodes exhibit an extremely low voltage(0.06/0.19/0.28 V) to achieve current densities of 10/50/100 mA cm^(-2) for energy-saving H_(2) production, which greatly reduces the electrolysis energy consumption. Moreover,DFT calculations further demonstrate that the introduction of Pt modulates the electronic structure of Rh and optimizes the d-band center, thus enhancing the adsorption and desorption of reactant/intermediates in the electrocatalytic reaction.
基金supported by the National Natural Science Foundation of China (No.52364022)the Natural Science Foundation of Guangxi Province,China (Nos.2023JJA160192 and 2021GXNSFAA220096)+1 种基金the Guangxi Science and Technology Major Project,China (No.AA23073018)the Guangxi Chongzuo Science and Technology Plan,China (No.2023ZY00503).
文摘With the application of resins in various fields, numerous waste resins that are difficult to treat have been produced. The industrial wastewater containing Cr(Ⅵ) has severely polluted soil and groundwater environments, thereby endangering human health. Therefore, in this paper, a novel functionalized mesoporous adsorbent PPR-Z was synthesized from waste amidoxime resin for adsorbing Cr(Ⅵ). The waste amidoxime resin was first modified with H3PO4 and ZnCl_(2), and subsequently, it was carbonized through slow thermal decomposition. The static adsorption of PPR-Z conforms to the pseudo-second-order kinetic model and Langmuir isotherm, indicating that the Cr(Ⅵ) adsorption by PPR-Z is mostly chemical adsorption and exhibits single-layer adsorption. The saturated adsorption capacity of the adsorbent for Cr(Ⅵ) could reach 255.86 mg/g. The adsorbent could effectively reduce Cr(Ⅵ) to Cr(Ⅲ) and decrease the toxicity of Cr(Ⅵ) during adsorption. PPR-Z exhibited Cr(Ⅵ) selectivity in electroplating wastewater. The main mechanisms involved in the Cr(Ⅵ) adsorption are the chemical reduction of Cr(Ⅵ) into Cr(Ⅲ) and electrostatic and coordination interactions. Preparation of PPR-Z not only solves the problem of waste resin treatment but also effectively controls Cr(Ⅵ) pollution and realizes the concept of “treating waste with waste”.
文摘Numerous decision-makers in politics,science,and business worldwide have acknowledged that hydrogen H_(2) will become one of the most important energy sources of the 21st century if the desired energy transition to carbon-free energy sources is to be taken seriously.Nevertheless,this transition in general and the introduction of H_(2) in particular is still progressing far too slowly.There are now countless projects worldwide,including several worth billions of US dollars,but we are still waiting for the breakthrough.There seem to be various reasons for this,not just one single or most important one.Purpose:In the overall context of global earth overheating(often downplayed as“climate change”),hydrogen H_(2) will undoubtedly play a decisive role as of now.The paper aims to identify the key challenges and propose solutions for establishing a sustainable value chain for market penetration of H_(2).Design/methodology/approach:This paper aims to shed light on the current situation using freely accessible publications from global management consultancies and the German government,as well as critical reporting.The problem of human behavior is also explained by the Novak Triangle.Findings:Most people have come to understand that anthropogenic global overheating can only be solved by new technologies(which cost money,time,and behavioral change)in production and application.Hydrogen H_(2) appears to be an essential part of the desired solution.Nevertheless,there are currently still numerous challenges and also concrete concerns worldwide,which partially cast the implementation in a questionable light.The findings suggest that establishing a demand and supply of H_(2) needs a comprehensive infrastructure,circular economy principles,and changes in consumer behavior and policy frameworks.The paper proposes solutions for addressing these challenges.Affected countries:The situation described here relates to Germany and the EU countries,but it is likely to be comparable,or at least similar,for many industrialized countries.The challenges and solutions proposed in this paper are relevant to countries worldwide that are transitioning to sustainable energy and transportation systems.Research/future/practical implications:As of 2024,it must be stated that the implementation of H_(2) is still progressing far too slowly,even in the“model country”Germany.There are still problems and stalling in many places.The biggest challenge seems to be the problem:without demand,there is no supply;without supply,there is no demand.This can then best be achieved with simple“out-of-the-box”solutions in mindset(see Novak triangle).The research implications of this paper include the need for further research on the challenges of establishing a sustainable value chain and the effectiveness of the proposed solutions.The future implications of this paper include the importance of establishing a sustainable value chain to mitigate climate change and reduce dependence on fossil fuels.The core point will become the collaboration across the entire value chain to establish a sustainable infrastructure for sustainable energy and transportation systems.Originality/value:Currently,there are virtually no scientific books that would present the overall context of the challenges.Therefore,only current surveys,market volumes,and challenges in environmental and working conditions can be described here.This paper contributes to the literature by analyzing the challenges of establishing a market model for hydrogen H_(2).The paper proposes solutions for addressing these challenges and shows difficulties.It provides valuable insights for policymakers,industry stakeholders,and researchers working towards a sustainable energy future.