Inefficient charge separation and limited light absorption are two critical issues associated with high‐efficiency photocatalytic H2production using TiO2.Surface defects within a certain concentration range in photoc...Inefficient charge separation and limited light absorption are two critical issues associated with high‐efficiency photocatalytic H2production using TiO2.Surface defects within a certain concentration range in photocatalyst materials are beneficial for photocatalytic activity.In this study,surface defects(oxygen vacancies and metal cation replacement defects)were induced with a facile and effective approach by surface doping with low‐cost transition metals(Co,Ni,Cu,and Mn)on ultrafine TiO2.The obtained surface‐defective TiO2exhibited a3–4‐fold improved activity compared to that of the original ultrafine TiO2.In addition,a H2production rate of3.4μmol/h was obtained using visible light(λ>420nm)irradiation.The apparent quantum yield(AQY)at365nm reached36.9%over TiO2‐Cu,significantly more than the commercial P25TiO2.The enhancement of photocatalytic H2production activity can be attributed to improved rapid charge separation efficiency andexpanded light absorption window.This hydrothermal treatment with transition metal was proven to be a very facile and effective method for obtaining surface defects.展开更多
Ultrathin small MoS2nanosheets exhibit a higher electrocatalytic activity for the hydrogen evolution reaction.However,strong interactions between MoS2layers may result in aggregation;together with the low conductivity...Ultrathin small MoS2nanosheets exhibit a higher electrocatalytic activity for the hydrogen evolution reaction.However,strong interactions between MoS2layers may result in aggregation;together with the low conductivity of MoS2,this may lower its electrocatalytic activity.In this paper we present a method that we developed to directly produce solid S,N co‐doped carbon(SNC)with a graphite structure and multiple surface groups through a hydrothermal route.When Na2MoO4was added to the reaction,polymolybdate could be anchored into the carbon materials via a chemical interaction that helps polymolybdate disperse uniformly into the SNC.After a high temperature treatment,polymolybdate transformed into MoS2at800°C for6h in a N2atmosphere at a heating rate of5°C/min,owing to S2?being released from the SNC during the treatment(denoted as MoS2/SNC‐800‐6h).The SNC effectively prevents MoS2from aggregating into large particles,and we successfully prepared highly dispersed MoS2in the SNC matrix.Electrochemical characterizations indicate that MoS2/SNC‐900‐12h exhibits a low onset potential of115mV and a low overpotential of237mV at a current density of10mA/cm2.Furthermore,MoS2/SNC‐900‐12h also had an excellent stability with only^2.6%decay at a current density of10mA/cm2after5000test cycles.展开更多
A 4.34 liter two stage air lift photobioreactor incorporating Anabaena variabilis ATCC29413 mutant PK84 was used to study H 2 production. Results showed that H 2 production increased with increasing light intensity fr...A 4.34 liter two stage air lift photobioreactor incorporating Anabaena variabilis ATCC29413 mutant PK84 was used to study H 2 production. Results showed that H 2 production increased with increasing light intensity from 47 μE/(m 2·s) up to 190 μE/(m 2·s), but that further increase of light intensity decreased the H 2 production because of the inhibition due to the high pO 2. The data also indicated that longer argon gas charge resulted in more H 2 produced due to the increase of nitrogenase activities and heterocyst frequency, and that more than 1.3 L net H 2 was produced from this computer controlled photobioreactor.展开更多
Background Chinese indigenous pigs are popular with consumers for their juiciness,flavour and meat quality,but they have lower meat production.Insulin-like growth factor 2(IGF2) is a maternally imprinted growth factor...Background Chinese indigenous pigs are popular with consumers for their juiciness,flavour and meat quality,but they have lower meat production.Insulin-like growth factor 2(IGF2) is a maternally imprinted growth factor that promotes skeletal muscle growth by regulating cell proliferation and differentiation.A single nucleotide polymorphism(SNP) within intron 3 of porcine IGF2 disrupts a binding site for the repressor,zinc finger BED-type containing 6(ZBED6),leading to up-regulation of IGF2 and causing major effects on muscle growth,heart size,and backfat thickness.This favorable mutation is common in Western commercial pig populations,but absent in most Chinese indigenous pig breeds.To improve meat production of Chinese indigenous pigs,we used cytosine base editor 3(CBE3)to introduce IGF2 intron3-C3071T mutation into porcine embryonic fibroblasts(PEFs) isolated from a male Liang Guang Small Spotted pig(LGSS),and single-cell clones harboring the desired mutation were selected for somatic cell nuclear transfer(SCNT) to generate the founder line of IGF2^(T/T) pigs.Results We found the heterozygous progeny IGF2^(C/T) pigs exhibited enhanced expression of IGF2,increased lean meat by 18%-36%,enlarged loin muscle area by 3%-17%,improved intramuscular fat(IMF) content by 18%-39%,marbling score by 0.75-1,meat color score by 0.53-1.25,and reduced backfat thickness by 5%-16%.The enhanced accumulation of intramuscular fat in IGF2^(C/T) pigs was identified to be regulated by the PI3K-AKT/AMPK pathway,which activated SREBP1 to promote adipogenesis.Conclusions We demonstrated the introduction of IGF2-intron3-C3071T in Chinese LGSS can improve both meat production and quality,and first identified the regulation of IMF deposition by IGF2 through SREBP1 via the PI3KAKT/AMPK signaling pathways.Our study provides a further understanding of the biological functions of IGF2and an example for improving porcine economic traits through precise base editing.展开更多
Designing a step-scheme(S-scheme)heterojunction photocatalyst with vacancy engineering is a reliable approach to achieve highly efficient photocatalytic H_(2)production activity.Herein,a hollow ZnO/ZnS S-scheme hetero...Designing a step-scheme(S-scheme)heterojunction photocatalyst with vacancy engineering is a reliable approach to achieve highly efficient photocatalytic H_(2)production activity.Herein,a hollow ZnO/ZnS S-scheme heterojunction with O and Zn vacancies(VO,Zn-ZnO/ZnS)is rationally constructed via ion-exchange and calcination treatments.In such a photocatalytic system,the hollow structure combined with the introduction of dual vacancies endows the adequate light absorption.Moreover,the O and Zn vacancies serve as the trapping sites for photo-induced electrons and holes,respectively,which are beneficial for promoting the photo-induced carrier separation.Meanwhile,the S-scheme charge transfer mechanism can not only improve the separation and transfer efficiencies of photo-induced carrier but also retain the strong redox capacity.As expected,the optimized VO,Zn-ZnO/ZnS heterojunction exhibits a superior photocatalytic H_(2) production rate of 160.91 mmol g^(-1)h^(-1),approximately 643.6 times and 214.5 times with respect to that obtained on pure ZnO and ZnS,respectively.Simultaneously,the experimental results and density functional theory calculations disclose that the photo-induced carrier transfer pathway follows the S-scheme heterojunction mechanism and the introduction of O and Zn vacancies reduces the surface reaction barrier.This work provides an innovative strategy of vacancy engineering in S-scheme heterojunction for solar-to-fuel energy conversion.展开更多
Soluble receptor for advanced glycation end products(sRAGE)acts as a decoy sequestering of RAGE ligands,thus preventing the activation of the ligand-RAGE axis linking human diseases.However,the molecular mechanisms un...Soluble receptor for advanced glycation end products(sRAGE)acts as a decoy sequestering of RAGE ligands,thus preventing the activation of the ligand-RAGE axis linking human diseases.However,the molecular mechanisms underlying sRAGE remain unclear.In this study,THP-1 monocytes were cultured in normal glucose(NG,5.5 mmol/L)and high glucose(HG,15 mmol/L)to investigate the effects of diabetesrelevant glucose concentrations on sRAGE and interleukin-1β(IL-1β)secretion.The modulatory effects of epigallocatechin gallate(EGCG)in response to HG challenge were also evaluated.HG enhanced intracellular reactive oxygen species(ROS)generation and RAGE expression.The secretion of sRAGE,including esRAGE and cRAGE,was reduced under HG conditions,together with the downregulation of a disintegrin and metallopeptidase 10(ADAM10)and nuclear factor erythroid 2-related factor 2(Nrf2)nuclear translocation.Mechanistically,the HG effects were counteracted by siRAGE and exacerbated by siNrf2.Chromatin immunoprecipitation results showed that Nrf2 binding to the ADAM10 promoter and HG interfered with this binding.Our data reinforce the notion that RAGE and Nrf2 might be sRAGE-regulating factors.Under HG conditions,the treatment of EGCG reduced ROS generation and RAGE activation.EGCG-stimulated cRAGE release was likely caused by the upregulation of the Nrf2-ADAM10 pathway.EGCG inhibited HG-mediated NLRP3 inflammasome activation at least partly by stimulating sRAGE,thereby reducing IL-1βrelease.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 development of an efficient artificial H_(2)O_(2) photosynthesis system is a challenging work using H_(2)O and O_(2) as starting materials.Herein,3D In_(2.77)S_(4) nanoflower precursor was in-situ deposited on K^(...The development of an efficient artificial H_(2)O_(2) photosynthesis system is a challenging work using H_(2)O and O_(2) as starting materials.Herein,3D In_(2.77)S_(4) nanoflower precursor was in-situ deposited on K^(+)-doped g-C_(3)N_(4)(KCN)nanosheets using a solvothermal method,then In_(2.77)S_(4)/KCN(IS/KCN)het-erojunction with an intimate interface was obtained after a calcination process.The investigation shows that the photocatalytic H_(2)O_(2) production rate of 50IS/KCN can reach up to 1.36 mmol g^(-1)h^(-1)without any sacrificial reagents under visible light irradiation,which is 9.2 times and 4.1 times higher than that of KCN and In_(2.77)S_(4)/respectively.The enhanced activity of the above composite can be mainly attributed to the S-scheme charge transfer route between KCN and In_(2.77)S_(4) according to density functional theory calculations,electron paramagnetic resonance and free radical capture tests,leading to an expanded light response range and rapid charge separation at their interface,as well as preserving the active electrons and holes for H_(2)O_(2) production.Besides,the unique 3D nanostructure and surface hydrophobicity of IS/KCN facilitate the diffusion and transportation of O_(2) around the active centers,the energy barriers of O_(2) protonation and H_(2)O_(2) desorption steps are ef-fectively reduced over the composite.In addition,this system also exhibits excellent light harvesting ability and stability.This work provides a potential strategy to explore a sustainable H_(2)O_(2) photo-synthesis pathway through the design of heterojunctions with intimate interfaces and desired reac-tion thermodynamics and kinetics.展开更多
Energy supply dominated by fossil energy has been and remains the main cause of carbon dioxide emissions,the major greenhouse gas leading to the current grave climate change challenges.Many technical pathways have bee...Energy supply dominated by fossil energy has been and remains the main cause of carbon dioxide emissions,the major greenhouse gas leading to the current grave climate change challenges.Many technical pathways have been proposed to address the challenges.Carbon capture and utilization(CCU) represents one of the approaches and thermochemical CO_(2) splitting driven by thermal energy is a subset of the CCU,which converts the captured CO_(2) into CO and makes it possible to achieve closed-loop carbon recirculation.Redox-active catalysts are among the most critical components of the thermochemical splitting cycles and perovskites are regarded as the most promising catalysts.Here we review the latest advancements in thermochemical cycles based on perovskites,covering thermodynamic principles,material modifications,reaction kinetics,oxygen pressure control,circular strategies,and demonstrations to provide a comprehensive overview of the topical area.Thermochemical cycles based on such materials require the consideration of trade-off between cost and efficiency,which is related to actual material used,operation mode,oxygen removal,and heat recovery.Lots of efforts have been made towards improving reaction rates,conversion efficiency and cycling stability,materials related research has been lacking-a key aspect affecting the performance across all above aspects.Double perovskites and composite perovskites arise recently as a potentially promising addition to material candidates.For such materials,more effective oxygen removal would be needed to enhance the overall efficiency,for which thermochemical or electrochemical oxygen pumps could contribute to efficient oxygen removal as well as serve as means for inert gas regeneration.The integration of thermochemical CO_(2) splitting process with downstream fuel production and other processes could reduce costs and increase efficiency of the technology.This represents one of the directions for the future research.展开更多
Steam reforming of long-chain hydrocarbon fuels for hydrogen production has received great attention for thermal management of the hypersonic vehicle and fuel-cell application.In this work,Pt catalysts supported on Ce...Steam reforming of long-chain hydrocarbon fuels for hydrogen production has received great attention for thermal management of the hypersonic vehicle and fuel-cell application.In this work,Pt catalysts supported on CeO_(2)and Tb-doped CeO_(2)were prepared by a precipitation method.The physical structure and chemical properties of the as-prepared catalysts were characterized by powder X-ray diffraction,scanning electron microscopy,transmission electron microscopy,Raman spectroscopy,H_(2)temperature programmed reduction,and X-ray photoelectron spectroscopy.The results show that Tb-doped CeO_(2)supported Pt possesses abundant surface oxygen vacancies,good inhibition of ceria sintering,and strong metal-support interaction compared with CeO_(2)supported Pt.The catalytic performance of hydrogen production via steam reforming of long-chain hydrocarbon fuels(n-dodecane)was tested.Compared with 2Pt/CeO_(2),2Pt/Ce_(0.9)Tb_(0.1)O_(2),and 2Pt/Ce_(0.5)Tb_(0.5)O_(2),the 2Pt/Ce_(0.7)Tb_(0.3)O_(2)has higher activity and stability for hydrogen production,on which the conversion of n-dodecane was maintained at about 53.2%after 600 min reaction under 700℃at liquid space velocity of 9 ml·g^(-1)·h^(-1).2Pt/CeO_(2)rapidly deactivated,the conversion of n-dodecane was reduced to only 41.6%after 600 min.展开更多
Carbon emission reduction and clean energy development are urgent demands for mankind in the coming decades.Exploring an efficient CO_(2) storage method can significantly reduce CO_(2) emissions in the short term.In t...Carbon emission reduction and clean energy development are urgent demands for mankind in the coming decades.Exploring an efficient CO_(2) storage method can significantly reduce CO_(2) emissions in the short term.In this study,we attempted to construct sediment samples with different residual CH_(4) hydrate amounts and reservoir conditions,and then investigate the potentials of both CO_(2) storage and enhanced CH_(4) recovery in depleted gas hydrate deposits in the permafrost and ocean zones,respectively.The results demonstrate that CO_(2) hydrate formation rate can be significantly improved due to the presence of residual hydrate seeds;However,excessive residual hydrates in turn lead to the decrease in CO_(2) storage efficiency.Affected by the T-P conditions of the reservoir,the storage amount of liquid CO_(2) can reach 8 times that of gaseous CO_(2),and CO_(2) stored in hydrate form reaches 2-4 times.Additionally,we noticed two other advantages of this method.One is that CO_(2) injection can enhance CH_(4) recovery rate and increases CH_(4) recovery by 10%-20%.The second is that hydrate saturation in the reservoir can be restored to 20%-40%,which means that the solid volume of the reservoir avoids serious shrinkage.Obviously,this is crucial for protecting the goaf stability.In summary,this approach is greatly promising for high-efficient CO_(2) storage and safe exploitation of gas hydrate.展开更多
In this study,Ni_(2)P/CdS composites were constructed by depositing non-precious metal co-catalyst Ni_(2)P on a one-dimensional network of CdS using a simple in-situ photodeposition method.The prepared photocatalysts ...In this study,Ni_(2)P/CdS composites were constructed by depositing non-precious metal co-catalyst Ni_(2)P on a one-dimensional network of CdS using a simple in-situ photodeposition method.The prepared photocatalysts promoted the decomposition of ethanol into high-value-added products while generating hydrogen.The composite photoanodes loaded with the Ni_(2)P co-catalysts showed significantly higher ethanol conversion and hydrogen production in the visible light region,which was almost three times higher than that of pure CdS.The main products of photocatalytic ethanol production are acetaldehyde(AA)and 2,3-butanediol(2,3-BDA).Compared with CdS,the selectivity of the composite photocatalysts for converting ethanol to acetaldehyde was significantly improved(62% to 78%).Characterization of the prepared photocatalysts confirmed that the loading of Ni_(2)P co-catalysts on CdS not only broadened the optical region of the catalysts for trapping light but also effectively promoted the separation and transfer of charge carriers,which significantly improved the photocatalytic efficiency of ethanol conversion and hydrogen production in the catalysts.It has been proven through Electron Paramagnetic Resonance testing that loading a Ni_(2)P co-catalyst on CdS is beneficial for the adsorption of hydroxyethyl radicals(*CH(OH)CH_(3)),thereby further improving the selectivity of acetaldehyde.This study plays an important role in the rational design of composite catalyst structures and the introduction of co-catalysts to improve catalyst performance,promote green chemistry,advocate a low-carbon society,and promote sustainable development.展开更多
Recent studies have indicated that the injection of carbon dioxide(CO_(2))can lead to increased oil recovery in fractured shale reservoirs following natural depletion.Despite advancements in understanding mass exchang...Recent studies have indicated that the injection of carbon dioxide(CO_(2))can lead to increased oil recovery in fractured shale reservoirs following natural depletion.Despite advancements in understanding mass exchange processes in subsurface formations,there remains a knowledge gap concerning the disparities in these processes between the matrix and fractures at the pore scale in formations with varying permeability.This study aims to experimentally investigate the CO_(2) diffusion behaviors and in situ oil recovery through a CO_(2) huff‘n’puff process in the Jimsar shale oil reservoir.To achieve this,we designed three matrix-fracture models with different permeabilities(0.074 mD,0.170 mD,and 0.466 mD)and experimented at 30 MPa and 91℃.The oil concentration in both the matrix and fracture was monitored using a low-field nuclear magnetic resonance(LF-NMR)technique to quantify in situ oil recovery and elucidate mass-exchange behaviors.The results showed that after three cycles of CO_(2) huff‘n’puff,the total recovery degree increased from 30.28%to 34.95%as the matrix permeability of the core samples increased from 0.074 to 0.466 mD,indicating a positive correlation between CO_(2) extraction efficiency and matrix permeability.Under similar fracture conditions,the increase in matrix permeability further promoted CO_(2) extraction efficiency during CO_(2) huff‘n’puff.Specifically,the increase in matrix permeability of the core had the greatest effect on the extraction of the first-cycle injection in large pores,which increased from 16.42%to 36.64%.The findings from our research provide valuable insights into the CO_(2) huff‘n’puff effects in different pore sizes following fracturing under varying permeability conditions,shedding light on the mechanisms of CO_(2)-enhanced oil recovery in fractured shale oil reservoirs.展开更多
Ammonia plays a crucial role in contemporary society,impacting medicine,agriculture,and the chemical industry.The conventional industrial synthesis of NH_(3) through the Haber-Bosch technique,carried out under severe ...Ammonia plays a crucial role in contemporary society,impacting medicine,agriculture,and the chemical industry.The conventional industrial synthesis of NH_(3) through the Haber-Bosch technique,carried out under severe reaction conditions,leads to substantial energy consumption and environmental pollution.It is thus imperative for NH_(3) synthesis methods to be investigated under more favorable conditions.Synthesis of ammonia by electrocatalysis can effectively reduce the environmental damage and other urgent problems,which is a promising solution.Metal-nitrogen series batteries(M-N batteries),such as metal-nitrogen gas batteries,metal-nitrogen oxide batteries and metal-oxynitride batteries have been regarded recently as an exemplar of concurrent NH_(3) synthesis and energy production.Nonetheless,the large-scale application of these batteries is still limited by numerous challenges are currently existing in building high-efficiency M-N batteries,including poor Faradic efficiency and low NH_(3) yield.Therefore,a comprehensive overview of M-N batteries is offered,specifically focusing on advanced strategies for designing highly efficient cathode catalysts in anticipation of future developments.The metal anodes,cathodic electro-reduction reactions,and design principles are encompassed in the discussion,offering detailed insights to enhance understanding.Mechanisms,feasibility analyses,technoeconomic assessments,device combinations,and comparative evaluations are delved into in the review,contributing to a thorough comprehension of diverse systems and their application potential.Perspectives and opportunities for future research directions are also delineated.展开更多
Constructing Z-scheme type photocatalyst is an efficient way to improve the charge separation efficiency and enhance the photocatalytic activity. In this report, the Cd:TiO2 nanoparticles are prepared via the sol-gel...Constructing Z-scheme type photocatalyst is an efficient way to improve the charge separation efficiency and enhance the photocatalytic activity. In this report, the Cd:TiO2 nanoparticles are prepared via the sol-gel route and employed as a starting material. When it was reduced by NaBH4 at 300°C,the surface oxygen vacancies were produced and Cd2+ was reduced into metal Cd0 nanoparticle(denoted as R-Cd:TiO2).Subsequently, the formed R-Cd:TiO2 was treated with thioureain the hydrothermal reaction. Through the decomposition of thiourea, the oxygen vacancies were refilled by S2- from thiourea to form S:TiO2/TiO2(d-TiO2) and Cd was partially converted into CdS to form CdS/Cd/d-TiO2 composite. The formed CdS/Cd/d-TiO2 composite exhibits improved photocatalytic activity. Under visible light irradiation(λ〉400 nm),the H2 production rate of CdS/Cd/d-TiO2 reaches 119 μmol h-1 with 50 mg of photocatalyst without any cocatalyst, which is about 200 and 60 times higher than that of S:TiO2/TiO2(0.57 μmol h-1), CdS(2.03 μmol h-1) and heterojunction CdS/d-TiO2(2.17 μmol h-1) materials, respectively. The results illustrate that metal Cd greatly promotes the charge separation efficiency due to the formation of Z-scheme type composite. In addition, the photocatalytic activity in the visible light region was dramatically enhanced due to the contribution of both CdS and d-TiO2. The method could be easily extended to other wide bandgap semiconductors for constructing visible light responsive Z-scheme type photocatalysts.展开更多
H2 with low CO concentration is produced via photocatalytic reforming of glucose (as a representative of biomass component) on metal/TiO2 catalyst (metals: Pt, Rh, Ru, Ir, Au, Ni, Cu). It is shown that the loaded meta...H2 with low CO concentration is produced via photocatalytic reforming of glucose (as a representative of biomass component) on metal/TiO2 catalyst (metals: Pt, Rh, Ru, Ir, Au, Ni, Cu). It is shown that the loaded metals generally enhance the rate of H2 production, while they depress the CO selectivity. Both H2 production and CO selectivity are strongly dependent on the kind of deposited metals on TiO2. For example, Rh/TiO2 catalyst is found to be most active for H2 production while with the most extremely low CO concentration from the photocatalytic reforming of glucose.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
Electrochemical synthesis of H_(2)O_(2) via a selective two-electron oxygen reduction reaction has emerged as an attractive alternative to the current energy-consuming anthraquinone process. Herein, the progress on el...Electrochemical synthesis of H_(2)O_(2) via a selective two-electron oxygen reduction reaction has emerged as an attractive alternative to the current energy-consuming anthraquinone process. Herein, the progress on electrocatalysts for H_(2)O_(2) generation, including noble metal, transition metalbased, and carbon-based materials, is summarized. At first, the design strategies employed to obtain electrocatalysts with high electroactivity and high selectivity are highlighted. Then, the critical roles of the geometry of the electrodes and the type of reactor in striking a balance to boost the H_(2)O_(2) selectivity and reaction rate are systematically discussed. After that, a potential strategy to combine the complementary properties of the catalysts and the reactor for optimal selectivity and overall yield is illustrated. Finally, the remaining challenges and promising opportunities for highefficient H_(2)O_(2) electrochemical production are highlighted for future studies.展开更多
We studied a method to prepare a novel titanium dioxide(TiO_(2))composite photocatalyst,starting from improving the separation efficiency of photogenerated electrons and holes.Regular TiO_(2)microspheres were prepared...We studied a method to prepare a novel titanium dioxide(TiO_(2))composite photocatalyst,starting from improving the separation efficiency of photogenerated electrons and holes.Regular TiO_(2)microspheres were prepared by sol-gel method and loaded onto Ti3C2Tx(Mxene).The high electrical conductivity of Mxene was utilized to transfer photogenerated electrons quickly and effectively prevent their recombination.By adjusting the addition amount of Mxene,the hydrogen production efficiency of the sample was greatly improved,and the maximum efficiency reached 135.2μmol·g^(-1)·h^(-1),which was twice that of pure TiO_(2).The nanocomposites were characterized by XRD,PL,TEM and SEM analysis and electrochemical methods,and the test proved that the improvement of hydrogen production efficiency was caused by the improvement of the separation efficiency of photogenerated electrons and holes.This work demonstrates the application of Mxene as a catalyst to improve efficiency and broadens the application prospects of Mxene.展开更多
Electrocatalytic water splitting for hydrogen production is hampered by the sluggish oxygen evolution reaction(OER)and large power consumption and replacing the OER with thermodynamically favourable reactions can impr...Electrocatalytic water splitting for hydrogen production is hampered by the sluggish oxygen evolution reaction(OER)and large power consumption and replacing the OER with thermodynamically favourable reactions can improve the energy conversion efficiency.Since iron corrodes easily and even self-corrodes to form magnetic iron oxide species and generate corrosion currents,a novel strategy to integrate the hydrogen evolution reaction(HER)with waste Fe upgrading reaction(FUR)is proposed and demonstrated for energy-efficient hydrogen production in neutral media.The heterostructured MoSe_(2)/MoO_(2) grown on carbon cloth(MSM/CC)shows superior HER performance to that of commercial Pt/C at high current densities.By replacing conventional OER with FUR,the potential required to afford the anodic current density of 10 m A cm^(-2)decreases by 95%.The HER/FUR overall reaction shows an ultralow voltage of 0.68 V for 10 m A cm^(-2)with a power equivalent of 2.69 k Wh per m^(3)H_(2).Additionally,the Fe species formed at the anode extract the Rhodamine B(Rh B)pollutant by flocculation and also produce nanosized magnetic powder and beneficiated Rh B for value-adding applications.This work demonstrates both energy-saving hydrogen production and pollutant recycling without carbon emission by a single system and reveals a new direction to integrate hydrogen production with environmental recovery to achieve carbon neutrality.展开更多
基金supported by the Double First‐rate Subject‐Food Science and Engineering Program of Hebei Province (2018SPGCA18)Young Tip‐top Talents Plan of Universities and Colleges in Hebei Province of China (BJ2017026)the Specific Foundation for Doctor in Hebei Agriculture University of China (ZD201709)~~
文摘Inefficient charge separation and limited light absorption are two critical issues associated with high‐efficiency photocatalytic H2production using TiO2.Surface defects within a certain concentration range in photocatalyst materials are beneficial for photocatalytic activity.In this study,surface defects(oxygen vacancies and metal cation replacement defects)were induced with a facile and effective approach by surface doping with low‐cost transition metals(Co,Ni,Cu,and Mn)on ultrafine TiO2.The obtained surface‐defective TiO2exhibited a3–4‐fold improved activity compared to that of the original ultrafine TiO2.In addition,a H2production rate of3.4μmol/h was obtained using visible light(λ>420nm)irradiation.The apparent quantum yield(AQY)at365nm reached36.9%over TiO2‐Cu,significantly more than the commercial P25TiO2.The enhancement of photocatalytic H2production activity can be attributed to improved rapid charge separation efficiency andexpanded light absorption window.This hydrothermal treatment with transition metal was proven to be a very facile and effective method for obtaining surface defects.
基金supported by the National Natural Science Foundation of China(21671011)Beijing High-Level Talent program~~
文摘Ultrathin small MoS2nanosheets exhibit a higher electrocatalytic activity for the hydrogen evolution reaction.However,strong interactions between MoS2layers may result in aggregation;together with the low conductivity of MoS2,this may lower its electrocatalytic activity.In this paper we present a method that we developed to directly produce solid S,N co‐doped carbon(SNC)with a graphite structure and multiple surface groups through a hydrothermal route.When Na2MoO4was added to the reaction,polymolybdate could be anchored into the carbon materials via a chemical interaction that helps polymolybdate disperse uniformly into the SNC.After a high temperature treatment,polymolybdate transformed into MoS2at800°C for6h in a N2atmosphere at a heating rate of5°C/min,owing to S2?being released from the SNC during the treatment(denoted as MoS2/SNC‐800‐6h).The SNC effectively prevents MoS2from aggregating into large particles,and we successfully prepared highly dispersed MoS2in the SNC matrix.Electrochemical characterizations indicate that MoS2/SNC‐900‐12h exhibits a low onset potential of115mV and a low overpotential of237mV at a current density of10mA/cm2.Furthermore,MoS2/SNC‐900‐12h also had an excellent stability with only^2.6%decay at a current density of10mA/cm2after5000test cycles.
文摘A 4.34 liter two stage air lift photobioreactor incorporating Anabaena variabilis ATCC29413 mutant PK84 was used to study H 2 production. Results showed that H 2 production increased with increasing light intensity from 47 μE/(m 2·s) up to 190 μE/(m 2·s), but that further increase of light intensity decreased the H 2 production because of the inhibition due to the high pO 2. The data also indicated that longer argon gas charge resulted in more H 2 produced due to the increase of nitrogenase activities and heterocyst frequency, and that more than 1.3 L net H 2 was produced from this computer controlled photobioreactor.
基金supported by the National Natural Science Foundation of China (3207269732030102)+2 种基金CARS-PIG-35R&D Programmes of Guangdong Province (2018B020203003)Laboratory of Lingnan Modern Agriculture Project (NZ2021006)。
文摘Background Chinese indigenous pigs are popular with consumers for their juiciness,flavour and meat quality,but they have lower meat production.Insulin-like growth factor 2(IGF2) is a maternally imprinted growth factor that promotes skeletal muscle growth by regulating cell proliferation and differentiation.A single nucleotide polymorphism(SNP) within intron 3 of porcine IGF2 disrupts a binding site for the repressor,zinc finger BED-type containing 6(ZBED6),leading to up-regulation of IGF2 and causing major effects on muscle growth,heart size,and backfat thickness.This favorable mutation is common in Western commercial pig populations,but absent in most Chinese indigenous pig breeds.To improve meat production of Chinese indigenous pigs,we used cytosine base editor 3(CBE3)to introduce IGF2 intron3-C3071T mutation into porcine embryonic fibroblasts(PEFs) isolated from a male Liang Guang Small Spotted pig(LGSS),and single-cell clones harboring the desired mutation were selected for somatic cell nuclear transfer(SCNT) to generate the founder line of IGF2^(T/T) pigs.Results We found the heterozygous progeny IGF2^(C/T) pigs exhibited enhanced expression of IGF2,increased lean meat by 18%-36%,enlarged loin muscle area by 3%-17%,improved intramuscular fat(IMF) content by 18%-39%,marbling score by 0.75-1,meat color score by 0.53-1.25,and reduced backfat thickness by 5%-16%.The enhanced accumulation of intramuscular fat in IGF2^(C/T) pigs was identified to be regulated by the PI3K-AKT/AMPK pathway,which activated SREBP1 to promote adipogenesis.Conclusions We demonstrated the introduction of IGF2-intron3-C3071T in Chinese LGSS can improve both meat production and quality,and first identified the regulation of IMF deposition by IGF2 through SREBP1 via the PI3KAKT/AMPK signaling pathways.Our study provides a further understanding of the biological functions of IGF2and an example for improving porcine economic traits through precise base editing.
文摘Designing a step-scheme(S-scheme)heterojunction photocatalyst with vacancy engineering is a reliable approach to achieve highly efficient photocatalytic H_(2)production activity.Herein,a hollow ZnO/ZnS S-scheme heterojunction with O and Zn vacancies(VO,Zn-ZnO/ZnS)is rationally constructed via ion-exchange and calcination treatments.In such a photocatalytic system,the hollow structure combined with the introduction of dual vacancies endows the adequate light absorption.Moreover,the O and Zn vacancies serve as the trapping sites for photo-induced electrons and holes,respectively,which are beneficial for promoting the photo-induced carrier separation.Meanwhile,the S-scheme charge transfer mechanism can not only improve the separation and transfer efficiencies of photo-induced carrier but also retain the strong redox capacity.As expected,the optimized VO,Zn-ZnO/ZnS heterojunction exhibits a superior photocatalytic H_(2) production rate of 160.91 mmol g^(-1)h^(-1),approximately 643.6 times and 214.5 times with respect to that obtained on pure ZnO and ZnS,respectively.Simultaneously,the experimental results and density functional theory calculations disclose that the photo-induced carrier transfer pathway follows the S-scheme heterojunction mechanism and the introduction of O and Zn vacancies reduces the surface reaction barrier.This work provides an innovative strategy of vacancy engineering in S-scheme heterojunction for solar-to-fuel energy conversion.
文摘Soluble receptor for advanced glycation end products(sRAGE)acts as a decoy sequestering of RAGE ligands,thus preventing the activation of the ligand-RAGE axis linking human diseases.However,the molecular mechanisms underlying sRAGE remain unclear.In this study,THP-1 monocytes were cultured in normal glucose(NG,5.5 mmol/L)and high glucose(HG,15 mmol/L)to investigate the effects of diabetesrelevant glucose concentrations on sRAGE and interleukin-1β(IL-1β)secretion.The modulatory effects of epigallocatechin gallate(EGCG)in response to HG challenge were also evaluated.HG enhanced intracellular reactive oxygen species(ROS)generation and RAGE expression.The secretion of sRAGE,including esRAGE and cRAGE,was reduced under HG conditions,together with the downregulation of a disintegrin and metallopeptidase 10(ADAM10)and nuclear factor erythroid 2-related factor 2(Nrf2)nuclear translocation.Mechanistically,the HG effects were counteracted by siRAGE and exacerbated by siNrf2.Chromatin immunoprecipitation results showed that Nrf2 binding to the ADAM10 promoter and HG interfered with this binding.Our data reinforce the notion that RAGE and Nrf2 might be sRAGE-regulating factors.Under HG conditions,the treatment of EGCG reduced ROS generation and RAGE activation.EGCG-stimulated cRAGE release was likely caused by the upregulation of the Nrf2-ADAM10 pathway.EGCG inhibited HG-mediated NLRP3 inflammasome activation at least partly by stimulating sRAGE,thereby reducing IL-1βrelease.
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.
文摘The development of an efficient artificial H_(2)O_(2) photosynthesis system is a challenging work using H_(2)O and O_(2) as starting materials.Herein,3D In_(2.77)S_(4) nanoflower precursor was in-situ deposited on K^(+)-doped g-C_(3)N_(4)(KCN)nanosheets using a solvothermal method,then In_(2.77)S_(4)/KCN(IS/KCN)het-erojunction with an intimate interface was obtained after a calcination process.The investigation shows that the photocatalytic H_(2)O_(2) production rate of 50IS/KCN can reach up to 1.36 mmol g^(-1)h^(-1)without any sacrificial reagents under visible light irradiation,which is 9.2 times and 4.1 times higher than that of KCN and In_(2.77)S_(4)/respectively.The enhanced activity of the above composite can be mainly attributed to the S-scheme charge transfer route between KCN and In_(2.77)S_(4) according to density functional theory calculations,electron paramagnetic resonance and free radical capture tests,leading to an expanded light response range and rapid charge separation at their interface,as well as preserving the active electrons and holes for H_(2)O_(2) production.Besides,the unique 3D nanostructure and surface hydrophobicity of IS/KCN facilitate the diffusion and transportation of O_(2) around the active centers,the energy barriers of O_(2) protonation and H_(2)O_(2) desorption steps are ef-fectively reduced over the composite.In addition,this system also exhibits excellent light harvesting ability and stability.This work provides a potential strategy to explore a sustainable H_(2)O_(2) photo-synthesis pathway through the design of heterojunctions with intimate interfaces and desired reac-tion thermodynamics and kinetics.
文摘Energy supply dominated by fossil energy has been and remains the main cause of carbon dioxide emissions,the major greenhouse gas leading to the current grave climate change challenges.Many technical pathways have been proposed to address the challenges.Carbon capture and utilization(CCU) represents one of the approaches and thermochemical CO_(2) splitting driven by thermal energy is a subset of the CCU,which converts the captured CO_(2) into CO and makes it possible to achieve closed-loop carbon recirculation.Redox-active catalysts are among the most critical components of the thermochemical splitting cycles and perovskites are regarded as the most promising catalysts.Here we review the latest advancements in thermochemical cycles based on perovskites,covering thermodynamic principles,material modifications,reaction kinetics,oxygen pressure control,circular strategies,and demonstrations to provide a comprehensive overview of the topical area.Thermochemical cycles based on such materials require the consideration of trade-off between cost and efficiency,which is related to actual material used,operation mode,oxygen removal,and heat recovery.Lots of efforts have been made towards improving reaction rates,conversion efficiency and cycling stability,materials related research has been lacking-a key aspect affecting the performance across all above aspects.Double perovskites and composite perovskites arise recently as a potentially promising addition to material candidates.For such materials,more effective oxygen removal would be needed to enhance the overall efficiency,for which thermochemical or electrochemical oxygen pumps could contribute to efficient oxygen removal as well as serve as means for inert gas regeneration.The integration of thermochemical CO_(2) splitting process with downstream fuel production and other processes could reduce costs and increase efficiency of the technology.This represents one of the directions for the future research.
基金supported by the Key Research and Design Program of Qinhuangdao(202101A005)the Science and Technology Project of Hebei Education Department(QN2023094)+2 种基金the Cultivation Project for Basic Research and Innovation of Yanshan University(2021LGQN028)the Project for Research and Development of Metal Catalysts for Photo-thermal Decomposition of Waste Plastics to Prepare Value-added Chemicals(x2023322)the Subsidy for Hebei Key Laboratory of Applied Chemistry after Operation Performance(22567616H).
文摘Steam reforming of long-chain hydrocarbon fuels for hydrogen production has received great attention for thermal management of the hypersonic vehicle and fuel-cell application.In this work,Pt catalysts supported on CeO_(2)and Tb-doped CeO_(2)were prepared by a precipitation method.The physical structure and chemical properties of the as-prepared catalysts were characterized by powder X-ray diffraction,scanning electron microscopy,transmission electron microscopy,Raman spectroscopy,H_(2)temperature programmed reduction,and X-ray photoelectron spectroscopy.The results show that Tb-doped CeO_(2)supported Pt possesses abundant surface oxygen vacancies,good inhibition of ceria sintering,and strong metal-support interaction compared with CeO_(2)supported Pt.The catalytic performance of hydrogen production via steam reforming of long-chain hydrocarbon fuels(n-dodecane)was tested.Compared with 2Pt/CeO_(2),2Pt/Ce_(0.9)Tb_(0.1)O_(2),and 2Pt/Ce_(0.5)Tb_(0.5)O_(2),the 2Pt/Ce_(0.7)Tb_(0.3)O_(2)has higher activity and stability for hydrogen production,on which the conversion of n-dodecane was maintained at about 53.2%after 600 min reaction under 700℃at liquid space velocity of 9 ml·g^(-1)·h^(-1).2Pt/CeO_(2)rapidly deactivated,the conversion of n-dodecane was reduced to only 41.6%after 600 min.
基金financially supported by the National Natural Science Foundation of China,China(22378424,52004136,22127812,U20B6005)the Science Foundation of China University of Petroleum Beijing(2462023BJRC017)Hunan Provincial Department of Education Scientific Research Project(22B0310).
文摘Carbon emission reduction and clean energy development are urgent demands for mankind in the coming decades.Exploring an efficient CO_(2) storage method can significantly reduce CO_(2) emissions in the short term.In this study,we attempted to construct sediment samples with different residual CH_(4) hydrate amounts and reservoir conditions,and then investigate the potentials of both CO_(2) storage and enhanced CH_(4) recovery in depleted gas hydrate deposits in the permafrost and ocean zones,respectively.The results demonstrate that CO_(2) hydrate formation rate can be significantly improved due to the presence of residual hydrate seeds;However,excessive residual hydrates in turn lead to the decrease in CO_(2) storage efficiency.Affected by the T-P conditions of the reservoir,the storage amount of liquid CO_(2) can reach 8 times that of gaseous CO_(2),and CO_(2) stored in hydrate form reaches 2-4 times.Additionally,we noticed two other advantages of this method.One is that CO_(2) injection can enhance CH_(4) recovery rate and increases CH_(4) recovery by 10%-20%.The second is that hydrate saturation in the reservoir can be restored to 20%-40%,which means that the solid volume of the reservoir avoids serious shrinkage.Obviously,this is crucial for protecting the goaf stability.In summary,this approach is greatly promising for high-efficient CO_(2) storage and safe exploitation of gas hydrate.
基金supported by the National Natural Science Foundation of China(22075197,22278290)the Shanxi Provincial Natural Science Foundation of China(202103021224079,201903D421081)the Research and Development Project of Key Core and Common Technology of Shanxi Province(20201102018)。
文摘In this study,Ni_(2)P/CdS composites were constructed by depositing non-precious metal co-catalyst Ni_(2)P on a one-dimensional network of CdS using a simple in-situ photodeposition method.The prepared photocatalysts promoted the decomposition of ethanol into high-value-added products while generating hydrogen.The composite photoanodes loaded with the Ni_(2)P co-catalysts showed significantly higher ethanol conversion and hydrogen production in the visible light region,which was almost three times higher than that of pure CdS.The main products of photocatalytic ethanol production are acetaldehyde(AA)and 2,3-butanediol(2,3-BDA).Compared with CdS,the selectivity of the composite photocatalysts for converting ethanol to acetaldehyde was significantly improved(62% to 78%).Characterization of the prepared photocatalysts confirmed that the loading of Ni_(2)P co-catalysts on CdS not only broadened the optical region of the catalysts for trapping light but also effectively promoted the separation and transfer of charge carriers,which significantly improved the photocatalytic efficiency of ethanol conversion and hydrogen production in the catalysts.It has been proven through Electron Paramagnetic Resonance testing that loading a Ni_(2)P co-catalyst on CdS is beneficial for the adsorption of hydroxyethyl radicals(*CH(OH)CH_(3)),thereby further improving the selectivity of acetaldehyde.This study plays an important role in the rational design of composite catalyst structures and the introduction of co-catalysts to improve catalyst performance,promote green chemistry,advocate a low-carbon society,and promote sustainable development.
基金National Natural Science Foundation of China via grant number 52174035,52304048China Postdoctoral Science Foundation(2022M722637)Research and Innovation Fund for Graduate Students of Southwest Petroleum University(2022KYCX026).
文摘Recent studies have indicated that the injection of carbon dioxide(CO_(2))can lead to increased oil recovery in fractured shale reservoirs following natural depletion.Despite advancements in understanding mass exchange processes in subsurface formations,there remains a knowledge gap concerning the disparities in these processes between the matrix and fractures at the pore scale in formations with varying permeability.This study aims to experimentally investigate the CO_(2) diffusion behaviors and in situ oil recovery through a CO_(2) huff‘n’puff process in the Jimsar shale oil reservoir.To achieve this,we designed three matrix-fracture models with different permeabilities(0.074 mD,0.170 mD,and 0.466 mD)and experimented at 30 MPa and 91℃.The oil concentration in both the matrix and fracture was monitored using a low-field nuclear magnetic resonance(LF-NMR)technique to quantify in situ oil recovery and elucidate mass-exchange behaviors.The results showed that after three cycles of CO_(2) huff‘n’puff,the total recovery degree increased from 30.28%to 34.95%as the matrix permeability of the core samples increased from 0.074 to 0.466 mD,indicating a positive correlation between CO_(2) extraction efficiency and matrix permeability.Under similar fracture conditions,the increase in matrix permeability further promoted CO_(2) extraction efficiency during CO_(2) huff‘n’puff.Specifically,the increase in matrix permeability of the core had the greatest effect on the extraction of the first-cycle injection in large pores,which increased from 16.42%to 36.64%.The findings from our research provide valuable insights into the CO_(2) huff‘n’puff effects in different pore sizes following fracturing under varying permeability conditions,shedding light on the mechanisms of CO_(2)-enhanced oil recovery in fractured shale oil reservoirs.
基金National Natural Science Foundation of China (22179065)Tianjin Graduate Research and Innovation Project (2022BKY018)。
文摘Ammonia plays a crucial role in contemporary society,impacting medicine,agriculture,and the chemical industry.The conventional industrial synthesis of NH_(3) through the Haber-Bosch technique,carried out under severe reaction conditions,leads to substantial energy consumption and environmental pollution.It is thus imperative for NH_(3) synthesis methods to be investigated under more favorable conditions.Synthesis of ammonia by electrocatalysis can effectively reduce the environmental damage and other urgent problems,which is a promising solution.Metal-nitrogen series batteries(M-N batteries),such as metal-nitrogen gas batteries,metal-nitrogen oxide batteries and metal-oxynitride batteries have been regarded recently as an exemplar of concurrent NH_(3) synthesis and energy production.Nonetheless,the large-scale application of these batteries is still limited by numerous challenges are currently existing in building high-efficiency M-N batteries,including poor Faradic efficiency and low NH_(3) yield.Therefore,a comprehensive overview of M-N batteries is offered,specifically focusing on advanced strategies for designing highly efficient cathode catalysts in anticipation of future developments.The metal anodes,cathodic electro-reduction reactions,and design principles are encompassed in the discussion,offering detailed insights to enhance understanding.Mechanisms,feasibility analyses,technoeconomic assessments,device combinations,and comparative evaluations are delved into in the review,contributing to a thorough comprehension of diverse systems and their application potential.Perspectives and opportunities for future research directions are also delineated.
基金financial support from the National Natural Science Foundation of China (21671011)Beijing High Talent Program+5 种基金Beijing Natural Science Foundation (KZ201710005002)China Postdoctoral Science FoundationBeijing Postdoctoral Research FoundationDongguan Program for International S&T Cooperationsupport from China Scholarship Councilsupported by the National Science Foundation (DMR-1506661, Feng P)
文摘Constructing Z-scheme type photocatalyst is an efficient way to improve the charge separation efficiency and enhance the photocatalytic activity. In this report, the Cd:TiO2 nanoparticles are prepared via the sol-gel route and employed as a starting material. When it was reduced by NaBH4 at 300°C,the surface oxygen vacancies were produced and Cd2+ was reduced into metal Cd0 nanoparticle(denoted as R-Cd:TiO2).Subsequently, the formed R-Cd:TiO2 was treated with thioureain the hydrothermal reaction. Through the decomposition of thiourea, the oxygen vacancies were refilled by S2- from thiourea to form S:TiO2/TiO2(d-TiO2) and Cd was partially converted into CdS to form CdS/Cd/d-TiO2 composite. The formed CdS/Cd/d-TiO2 composite exhibits improved photocatalytic activity. Under visible light irradiation(λ〉400 nm),the H2 production rate of CdS/Cd/d-TiO2 reaches 119 μmol h-1 with 50 mg of photocatalyst without any cocatalyst, which is about 200 and 60 times higher than that of S:TiO2/TiO2(0.57 μmol h-1), CdS(2.03 μmol h-1) and heterojunction CdS/d-TiO2(2.17 μmol h-1) materials, respectively. The results illustrate that metal Cd greatly promotes the charge separation efficiency due to the formation of Z-scheme type composite. In addition, the photocatalytic activity in the visible light region was dramatically enhanced due to the contribution of both CdS and d-TiO2. The method could be easily extended to other wide bandgap semiconductors for constructing visible light responsive Z-scheme type photocatalysts.
基金the National Natural Science Foundation of China (Grant No. 20403018, 20503034)National Basic Research Program of China (Grant No. 2003CB214504)Knowledge Innovation Program of the Chinese Academy of Sciences (DICP K2006E2)
文摘H2 with low CO concentration is produced via photocatalytic reforming of glucose (as a representative of biomass component) on metal/TiO2 catalyst (metals: Pt, Rh, Ru, Ir, Au, Ni, Cu). It is shown that the loaded metals generally enhance the rate of H2 production, while they depress the CO selectivity. Both H2 production and CO selectivity are strongly dependent on the kind of deposited metals on TiO2. For example, Rh/TiO2 catalyst is found to be most active for H2 production while with the most extremely low CO concentration from the photocatalytic reforming of glucose.
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 (22279036)。
文摘Electrochemical synthesis of H_(2)O_(2) via a selective two-electron oxygen reduction reaction has emerged as an attractive alternative to the current energy-consuming anthraquinone process. Herein, the progress on electrocatalysts for H_(2)O_(2) generation, including noble metal, transition metalbased, and carbon-based materials, is summarized. At first, the design strategies employed to obtain electrocatalysts with high electroactivity and high selectivity are highlighted. Then, the critical roles of the geometry of the electrodes and the type of reactor in striking a balance to boost the H_(2)O_(2) selectivity and reaction rate are systematically discussed. After that, a potential strategy to combine the complementary properties of the catalysts and the reactor for optimal selectivity and overall yield is illustrated. Finally, the remaining challenges and promising opportunities for highefficient H_(2)O_(2) electrochemical production are highlighted for future studies.
基金Funded by the National Natural Science Foundation of China (No.52003212)。
文摘We studied a method to prepare a novel titanium dioxide(TiO_(2))composite photocatalyst,starting from improving the separation efficiency of photogenerated electrons and holes.Regular TiO_(2)microspheres were prepared by sol-gel method and loaded onto Ti3C2Tx(Mxene).The high electrical conductivity of Mxene was utilized to transfer photogenerated electrons quickly and effectively prevent their recombination.By adjusting the addition amount of Mxene,the hydrogen production efficiency of the sample was greatly improved,and the maximum efficiency reached 135.2μmol·g^(-1)·h^(-1),which was twice that of pure TiO_(2).The nanocomposites were characterized by XRD,PL,TEM and SEM analysis and electrochemical methods,and the test proved that the improvement of hydrogen production efficiency was caused by the improvement of the separation efficiency of photogenerated electrons and holes.This work demonstrates the application of Mxene as a catalyst to improve efficiency and broadens the application prospects of Mxene.
基金financially supported by the Key Research and Development Program of Hubei Province (2021BAA208)the National Natural Science Foundation of China (52002294,51974208 and U2003130)+3 种基金the Young Top-notch Talent Cultivation Program of Hubei ProvinceKnowledge Innovation Program of Wuhan-Shuguang Project (2022010801020364)the City University of Hong Kong Strategic Research Grant (SRG) (7005505)the City University of Hong Kong Donation Research Grant (DONRMG 9229021)。
文摘Electrocatalytic water splitting for hydrogen production is hampered by the sluggish oxygen evolution reaction(OER)and large power consumption and replacing the OER with thermodynamically favourable reactions can improve the energy conversion efficiency.Since iron corrodes easily and even self-corrodes to form magnetic iron oxide species and generate corrosion currents,a novel strategy to integrate the hydrogen evolution reaction(HER)with waste Fe upgrading reaction(FUR)is proposed and demonstrated for energy-efficient hydrogen production in neutral media.The heterostructured MoSe_(2)/MoO_(2) grown on carbon cloth(MSM/CC)shows superior HER performance to that of commercial Pt/C at high current densities.By replacing conventional OER with FUR,the potential required to afford the anodic current density of 10 m A cm^(-2)decreases by 95%.The HER/FUR overall reaction shows an ultralow voltage of 0.68 V for 10 m A cm^(-2)with a power equivalent of 2.69 k Wh per m^(3)H_(2).Additionally,the Fe species formed at the anode extract the Rhodamine B(Rh B)pollutant by flocculation and also produce nanosized magnetic powder and beneficiated Rh B for value-adding applications.This work demonstrates both energy-saving hydrogen production and pollutant recycling without carbon emission by a single system and reveals a new direction to integrate hydrogen production with environmental recovery to achieve carbon neutrality.