1.Roles of biomass and bioenergy in solar energy storage Biomass comprises plant-based material,for example,wood,microalgae,energy crops,and agro-forestry residues,as well as organic waste from industries,farms,and ho...1.Roles of biomass and bioenergy in solar energy storage Biomass comprises plant-based material,for example,wood,microalgae,energy crops,and agro-forestry residues,as well as organic waste from industries,farms,and households,and plays a key role in solar energy capture and storage.展开更多
Owing to their high luminous efficiency and tunable emission in both red light and far-red light regions,Mn^(4+)ion-activated phosphors have appealed significant interest in photoelectric and energy conversion devices...Owing to their high luminous efficiency and tunable emission in both red light and far-red light regions,Mn^(4+)ion-activated phosphors have appealed significant interest in photoelectric and energy conversion devices such as white light emitting diode(W-LED),plant cultivation LED,and temperature thermometer.Up to now,Mn^(4+)has been widely introduced into the lattices of various inorganic hosts for brightly redemitting phosphors.However,how to correlate the structure-activity relationship between host framework,luminescence property,and photoelectric device is urgently demanded.In this review,we thoroughly summarize the recent advances of Mn^(4+)doped phosphors.Meanwhile,several strategies like co-doping and defect passivation for improving Mn^(4+)emission are also discussed.Most importantly,the relationship between the protocols for tailoring the structures of Mn^(4+)doped phosphors,increased luminescence performance,and the targeted devices with efficient photoelectric and energy conversion efficiency is deeply correlated.Finally,the challenges and perspectives of Mn^(4+)doped phosphors for practical applications are anticipated.We cordially anticipate that this review can deliver a deep comprehension of not only Mn^(4+)luminescence mechanism but also the crystal structure tailoring strategy of phosphors,so as to spur innovative thoughts in designing advanced phosphors and deepening the applications.展开更多
Biomass-to-ethylene glycol is an effective means to achieve high-value utilisation of cellulose but is hindered by low conversion efficiency and poor catalyst activity and stability.Glucose and cellobiose are derivati...Biomass-to-ethylene glycol is an effective means to achieve high-value utilisation of cellulose but is hindered by low conversion efficiency and poor catalyst activity and stability.Glucose and cellobiose are derivatives of cellulose conversion to ethylene glycol,and it is found that studying the reaction process of both can help to understand the reaction mechanism of cellulose.It is desirable to develop a reusable,highly active catalyst to convert cellulose into ethylene glycol.This ideal catalyst might have one or more active sites described the conversion steps above.Here,we discuss the catalyst development of celluloseto-ethylene glycol,including tungsten,tin,lanthanide,and other transition metal catalysts,and special attention is given to the reaction mechanism and kinetics for preparing ethylene glycol from cellulose,and the economic advantages of biomass-to-ethylene glycol are briefly introduced.The insights given in this review will facilitate further development of efficient catalysts,for addressing the global energy crisis and climate change related to the use of fossil fuels.展开更多
Aerogel nanoporous materials possess high porosity, high specific surface area, and extremely low density due to their unique nanoscale network structure. Moreover, their effective thermal conductivity is very low, ma...Aerogel nanoporous materials possess high porosity, high specific surface area, and extremely low density due to their unique nanoscale network structure. Moreover, their effective thermal conductivity is very low, making them a new type of lightweight and highly efficient nanoscale super-insulating material. However, prediction of their effective thermal conductivity is challenging due to their uneven pore size distribution. To investigate the internal heat transfer mechanism of aerogel nanoporous materials, this study constructed a cross-aligned and cubic pore model(CACPM) based on the actual pore arrangement of Si O2aerogel. Based on the established CACPM, the effective thermal conductivity expression for the aerogel was derived by simultaneously considering gas-phase heat conduction, solid-phase heat conduction, and radiative heat transfer. The derived expression was then compared with available experimental data and the Wei structure model. The results indicate that, according to the model established in this study for the derived thermal conductivity formula of silica aerogel, for powdery silica aerogel under the conditions of T = 298 K, a_(2)= 0.85, D_1= 90 μm, ρ = 128 kg/m^(3), within the pressure range of 0–105Pa, the average deviation between the calculated values and experimental values is 10.51%. In the pressure range of 103–104Pa, the deviation between calculated values and experimental values is within 4%. Under these conditions, the model has certain reference value in engineering verification. This study also makes a certain contribution to the research of aerogel thermal conductivity heat transfer models and calculation formulae.展开更多
Wet flue gas desulphurization technology is widely used in the industrial process for its capability of efficient pollution removal.The desulphurization control system,however,is subjected to complex reaction mechanis...Wet flue gas desulphurization technology is widely used in the industrial process for its capability of efficient pollution removal.The desulphurization control system,however,is subjected to complex reaction mechanisms and severe disturbances,which make for it difficult to achieve certain practically relevant control goals including emission and economic performances as well as system robustness.To address these challenges,a new robust control scheme based on uncertainty and disturbance estimator(UDE)and model predictive control(MPC)is proposed in this paper.The UDE is used to estimate and dynamically compensate acting disturbances,whereas MPC is deployed for optimal feedback regulation of the resultant dynamics.By viewing the system nonlinearities and unknown dynamics as disturbances,the proposed control framework allows to locally treat the considered nonlinear plant as a linear one.The obtained simulation results confirm that the utilization of UDE makes the tracking error negligibly small,even in the presence of unmodeled dynamics.In the conducted comparison study,the introduced control scheme outperforms both the standard MPC and PID(proportional-integral-derivative)control strategies in terms of transient performance and robustness.Furthermore,the results reveal that a lowpass-filter time constant has a significant effect on the robustness and the convergence range of the tracking error.展开更多
The development of rechargeable magnesium(Mg) batteries is of practical significance to upgrade the electric energy storage devices due to exceptional capacity and abundant resources of Mg-metal anode.However,the reve...The development of rechargeable magnesium(Mg) batteries is of practical significance to upgrade the electric energy storage devices due to exceptional capacity and abundant resources of Mg-metal anode.However,the reversible Mg electrochemistry suffers from unsatisfied rate capability and lifespan,mainly caused by non-uniform distribution of electrodeposits.In this work,a fresh design concept of threedimensional carbon cloths scaffolds is proposed to overcome the uncontrollable Mg growth via homogenizing electric field and improving magnesiophilicity.A microscopic smooth and nitrogen-containing defective carbonaceous layer is constructed through a facile pyrolysis of ZIF8 on carbon cloths.As revealed by finite element simulation and DFT calculation results,the smooth surface endows with uniform electric field distribution and simultaneously the nitrogen-doping species enable good magnesiophilicity of scaffolds.The fine and uniform Mg nucleus as well as the inner electrodeposit behavior are also disclosed.As a result,an exceptional cycle life of 500 cycles at 4.0 mA cm^(-2) and 4.0 mA h cm^(-2) is firstly realized to our best knowledge.Besides,the functional scaffolds can be cycled for over 2200 h at 2.0 mA cm^(-2) under a normalized capacity of 5.0 mA h cm^(-2),far exceeding previous results.This work offers an effective approach to enable the full potential of carbon cloths-based scaffolds towards metal storage for next generation battery applications.展开更多
The paper presents an energy performance assessment of CO2 removal for crude synthetic natural gas (SNG) upgrade by Selexol absorption process. A simplified process simulation of the Selexol process concerning power...The paper presents an energy performance assessment of CO2 removal for crude synthetic natural gas (SNG) upgrade by Selexol absorption process. A simplified process simulation of the Selexol process concerning power requirement and separation performance was developed. The assessment indicates that less pressure difference between crude SNG and absorption pressure favors the energy performance of CO2 removal process. When both crude SNG and absorption pressures are 20 bar, CO2 removal process has the best energy performance. The optimal specific power consumption of the CO2 removal process is 566 kJ/kgCO2. The sensitivity analysis shows that the CO2 removal efficiency would significantly influence the total power consumption of the removal process, as well as higher heating value (HHV) and CO2 content in SNG. However, the specific power consumption excluding crude SNG and SNG compressions changes little with the variance of CO2 removal efficiency. If by-product CO2 is compressed for CO2 capture, the process would turn into a CO2-sink for the atmosphere. Correspondingly, an increase of 281 kJ/kgCO2 in specific power consumption is required for compressing the separated CO2.展开更多
As the development of city economy,Zhongdong River in Hangzhou was seriously polluted,with the worst water quality.In order to obtain the effect of water diversion and distribution from Qiantang River on the water qua...As the development of city economy,Zhongdong River in Hangzhou was seriously polluted,with the worst water quality.In order to obtain the effect of water diversion and distribution from Qiantang River on the water quality of Zhongdong River,7-year continuous monitoring was conducted,which was at the fixed stations before and after the water diversion and distribution.After the water diversion project,the dissolved oxygen concentration of the river water was one to two times higher than before,and the ammonia nitrogen and total phosphorus decreased by 60%and 65%,respectively.When increased the amount of water diversion,the dissolved oxygen concentration of the river water elevated by 13%,and the ammonia nitrogen,total phosphorus and potassium permanganate index decreased by 8%,3%and 14%,respectively.The reason for the river water pollution was contributed to the combined sewer system and riverway sludge,especially during the rainfall,the dissolved oxygen concentration of Zhongdong River sharply declined by 95%,while the ammonia nitrogen and total phosphorus increased by 90%and 87%,respectively.The research results could provide theoretic basis for sustainable improvement of Zhongdong River water quality and river management department making the related regulations and policies.展开更多
The construction of high-efficiency and low-cost non-noble metal bifunctional electrocatalysts for water electrolysis is crucial for commercial large-scale application of hydrogen energy.Here,we report a novel strateg...The construction of high-efficiency and low-cost non-noble metal bifunctional electrocatalysts for water electrolysis is crucial for commercial large-scale application of hydrogen energy.Here,we report a novel strategy with erbiumdoped NiCoP nanowire arrays in situ grown on conductive nickel foam(Er-NiCoP/NF).Significantly,the developed electrode shows exceptional bifunctional catalytic activity,which only requires overpotentials of 46 and 225 mV to afford a current density of 10 mAcm^(−2) for the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OER),respectively.Density functional theory calculations reveal that the appropriate Er incorporation into the NiCoP lattice can significantly modulate the electronic structure with the d-band centers of Ni and Co atoms by shifting to lower energies with respect to the Fermi level,and optimize the Gibbs free energies of HER/OER intermediates,thereby accelerating water-splitting kinetics.When assembled as a solar-driven overall water-splitting electrolyzer,the as-prepared electrode shows a high and stable solar-to-hydrogen efficiency of 19.6%,indicating its potential for practical storage of intermittent energy.展开更多
Battery safety has attracted considerable attention worldwide due to the rapid development of wearable electronics and the steady increase in the production and use of electric vehicles.As battery failures are often a...Battery safety has attracted considerable attention worldwide due to the rapid development of wearable electronics and the steady increase in the production and use of electric vehicles.As battery failures are often associated with mechanical-thermal coupled behaviors,protective shielding materials with excellent mechanical robustness and flame-retardant properties are highly desired to mitigate thermal runaway.However,most of the thermal insulating materials are not strong enough to protect batteries from mechanical abuse,which is one of the most critical scenarios with catastrophic consequences.Here,inspired by wood,we have developed an effective approach to engineer a hierarchical nanocomposite via self-assembly of calcium silicate hydrate and polyvinyl alcohol polymer chains(referred as CSH wood).The versatile protective material CSH wood demonstrates an unprecedented combination of light weight(0.018 g cm-3),high stiffness(204 MPa in the axial direction),negative Poisson's ratio(-0.15),remarkable toughness(6.67×105 J m-3),superior thermal insulation(0.0204 W m-1 K-1 in the radial direction),and excellent fire retardancy(UL94-V0).When applied as a protective cover or a protective layer within battery packages,the tough CSH wood can resist high-impact load and block heat diffusion to block or delay the spread of fire,therefore significantly reducing the risk of property damage or bodily injuries caused by battery explosions.This work provides new pathways for fabricating advanced thermal insulating materials with large scalability and demonstrates great potential for the protection of electronic devices.展开更多
In this work,a“cyclopentanone-vanillin”strategy was proposed for the preparation of jet fuel range cycloalkanes from lignocellulose-derived ketones and lignin-derived aldehydes via aldol condensation and hydrodeoxyg...In this work,a“cyclopentanone-vanillin”strategy was proposed for the preparation of jet fuel range cycloalkanes from lignocellulose-derived ketones and lignin-derived aldehydes via aldol condensation and hydrodeoxygenation(HDO).Ethanolamine lactate ionic liquid(LAIL)exhibited excellent catalytic activity in the aldol condensation of cyclopentanone and vanillin.Desired mono-condensation and bicondensation products were obtained with yield of 95.2%at 100℃.It is found that the synergy effects between amino group of ethanolamine and hydroxyl group of lactic acid play a key role in the aldol condensation.The condensation products were converted into cycloalkanes by HDO over 5%Pd/Nb_(2)O_(5)catalyst.The density of the obtained HDO products is 0.89 g/cm^(3)and the freezing point is lower than-60℃.These results suggest that the resulted cycloalkanes can be used as additives to improve the density and low-temperature fluidity of the jet fuels.展开更多
The laminar combustion characteristics of CH_(4)/air premixed flames with CO_(2) addition are systemically studied.Experimental measurements and numerical simulations of the laminar burning velocity(LBV)are performed ...The laminar combustion characteristics of CH_(4)/air premixed flames with CO_(2) addition are systemically studied.Experimental measurements and numerical simulations of the laminar burning velocity(LBV)are performed in CH_(4)/CO_(2)/Air flames with various CO_(2) doping ratio under equivalence ratios of 1.0–1.4.GRI 3.0 mech and Aramco mech are employed for predicting LBV,adiabatic flame temperature(AFT),important intermediate radicals(CH_(3),H,OH,O)and NO_(x) emissions(NO,NO_(2),N2O),as well as the sensitivity analysis is also conducted.The detail analysis of experiment and simulation reveals that as the CO_(2) addition increases from 0%to 40%,the LBVs and AFTs decrease monotonously.Under the same CO_(2) doping ratio,the LBVs and AFTs increase first and then decrease with the increase of equivalence ratio,and the maximum of LBV is reached at equivalence ratio of 1.05.The mole fraction tendency of important intermediates and NO_(x) with equivalence ratio and CO_(2) doping ratio are similar to the LBVs and AFTs.Reaction H+O_(2)⇔O+OH is found to be responsible for the promotion of the generation of important intermediates and NO_(x) under the equivalence ratios and CO_(2) addition through sensitivity analysis.The sensitivity coefficients of elementary reactions that the increasing of CO_(2) doping ratio promotes or inhibits formation of intermediate radicals and NO_(x) decreases.展开更多
Cu-Li battery with Cu metal cathode and Li metal anode is a candidate for next-generation energy storage system.While self-discharge of the battery can be suppressed with an anion exchange membrane,the voltage polariz...Cu-Li battery with Cu metal cathode and Li metal anode is a candidate for next-generation energy storage system.While self-discharge of the battery can be suppressed with an anion exchange membrane,the voltage polarization depends strongly on the electrolyte.Specifically,when an electrolyte with 3 M LiTFSI(lithium bis(trifluoromethanesulfonyl)imide)in dimethyl carbonate(DMC)is used,overpotential increases with cycling.In this work,we reveal why the voltage polarization changes,and reduce and stabilize it by replacing DMC solvent with a mixed solvent composed of dimethoxyethane(DME)and propylene carbonate(PC).The new electrolyte has higher ionic conductivity and stable solvation structure with more free TFSI-anions upon cycling,which also facilitates uniform plating of metal ions on the metal electrodes.These characteristics enable a stable Cu-Li battery with minimal change in overpotential for more than 1500 cycles at a current density of 2 m A cm^(-2).展开更多
Since the utilization of abundant biomass to develop advanced materials has become an utmost priority in recent years,we developed two sustainable routes(i.e.,the impregnation method and the one-pot synthesis)to prepa...Since the utilization of abundant biomass to develop advanced materials has become an utmost priority in recent years,we developed two sustainable routes(i.e.,the impregnation method and the one-pot synthesis)to prepare the hydrochar-supported catalysts and tested its catalytic performance on the reductive amination.Several techniques,such as TEM,XRD and XPS,were adopted to characterize the structural and catalytic features of samples.Results indicated that the impregnation method favors the formation of outer-sphere surface complexes with porous structure as well as well-distributed metallic nanoparticles,while the one-pot synthesis tends to form the inner-sphere surface complexes with relatively smooth appearance and amorphous metals.This difference explains the better activity of catalysts prepared by the impregnation method which can selectively convert benzaldehyde to benzylamine with an excellent yield of 93.7%under the optimal reaction conditions;in contrast,the catalyst prepared by the one-pot synthesis only exhibits a low selectivity near to zero.Furthermore,the gram-scale test catalyzed by the same catalysts exhibits a similar yield of benzylamine in comparison to its smaller scale,which is comparable to the previously reported heterogeneous noble-based catalysts.More surprisingly,the prepared catalysts can be expediently recycled by a magnetic bar and remain the satisfying catalytic activity after reusing up to five times.In conclusion,these developed catalysts enable the synthesis of functional amines with excellent selectivity and carbon balance,proving cost-effective and sustainable access to the wide application of reductive amination.展开更多
The next-generation energy storage systems such as fuel cells,metal-air batteries,and alkali metal(Li,Na)-chalcogen(S,Se)batteries have received increasing attention owing to their high energy density and low cost.How...The next-generation energy storage systems such as fuel cells,metal-air batteries,and alkali metal(Li,Na)-chalcogen(S,Se)batteries have received increasing attention owing to their high energy density and low cost.However,one of the main obstacles of these systems is the poor reaction kinetics in the involved chemical reactions.Therefore,it is essential to incorporate suitable and efficient catalysts into the cell.These years,single-atom catalysts(SACs)are emerging as a frontier in catalysis due to their maximum atom efficiency and unique reaction selectivity.For SACs fabrication,metal-organic frameworks(MOFs)have been confirmed as promising templates or precursors due to their high metal loadings,structural adjustability,porosity,and tailorable catalytic site.In this review,we summarize effective strategies for fabricating SACs by MOFs with corresponding advanced characterization techniques and illustrate the key role of MOFs-based SACs in these batteries by explaining their reaction mechanisms and challenges.Finally,current applications,prospects,and opportunities for MOFs-based SACs in energy storage systems are discussed.展开更多
Air-stable layered structured cathodes with high voltage and good cycling stability are highly desired for the practical application of Na-ion batteries.Herein,we report a P2-Na_(2/3)Ni_(2/3)Te_(1/3)O_(2) cathode that...Air-stable layered structured cathodes with high voltage and good cycling stability are highly desired for the practical application of Na-ion batteries.Herein,we report a P2-Na_(2/3)Ni_(2/3)Te_(1/3)O_(2) cathode that is stable in ambient air with an average operating voltage of~3.8 V,demonstrating excellent cycling stability with a capacity retention of more than 92.7%after 500 cycles at 20 mA g^(-1) and good rate capability with 91.9%capacity utilization at 500 mA g^(-1) with respect to capacity at 5 mA g^(-1) between 2.0 and 4.0 V.When the upper cutoff voltage is increased to 4.4 V,P2-Na_(2/3)Ni_(2/3)Te_(1/3)O_(2) delivers a reversible capacity of 71.9 mAh g^(-1) and retains 91.8%of the capacity after 100 cycles at 20 mA g^(-1).The charge compensation during charge/discharge is mainly due to the redox couple of Ni^(2+)/Ni^(3+)in the host with a small amount of contribution from oxygen.The stable structure of the material without phase transformation and with small volume change during charge-discharge allows it to give excellent cycle performance especially when the upper cutoff voltage is not higher than 4.2 V.展开更多
During boreal winter,the invasion of cold air can lead to remarkable temperature drops in East Asia which can result in serious socioeconomic impacts.Here,we find that the intensity of strong synoptic cold days in the...During boreal winter,the invasion of cold air can lead to remarkable temperature drops in East Asia which can result in serious socioeconomic impacts.Here,we find that the intensity of strong synoptic cold days in the East China Sea and Indochina Peninsula are increasing.The enhanced synoptic cold days in these two regions are attributed to surface warming over the South China Sea and Philippine Sea(SCSPS).The oceanic forcing of the SCSPS on the synoptic cold days in the two regions is verified by numerical simulation.The warming of the SCSPS enhances the baroclinicity,which intensifies meridional wind and cold advection on synoptic timescales.This leads to a more extended region that is subject to the influence of cold invasion.展开更多
Safe batteries are the basis for next-generation application scenarios such as portable energy storage devices and electric vehicles,which are crucial to achieving carbon neutralization.Electrolytes,separators,and ele...Safe batteries are the basis for next-generation application scenarios such as portable energy storage devices and electric vehicles,which are crucial to achieving carbon neutralization.Electrolytes,separators,and electrodes as main components of lithium batteries strongly affect the occurrence of safety accidents.Responsive materials,which can respond to external stimuli or environmental change,have triggered extensive attentions recently,holding great promise in facilitating safe and smart batteries.This review thoroughly discusses recent advances regarding the construction of high-safety lithium batteries based on internal thermal-responsive strategies,together with the corresponding changes in electrochemical performance under external stimulus.Furthermore,the existing challenges and outlook for the design of safe batteries are presented,creating valuable insights and proposing directions for the practical implementation of safe lithium batteries.展开更多
The use of lithium-sulfur batteries under high sulfur loading and low electrolyte concentrations is severely restricted by the detrimental shuttling behavior of polysulfides and the sluggish kinetics in redox processe...The use of lithium-sulfur batteries under high sulfur loading and low electrolyte concentrations is severely restricted by the detrimental shuttling behavior of polysulfides and the sluggish kinetics in redox processes.Two-dimensional(2D)few layered black phosphorus with fully exposed atoms and high sulfur affinity can be potential lithium-sulfur battery electrocatalysts,which,however,have limitations of restricted catalytic activity and poor electrochemical/chemical stability.To resolve these issues,we developed a multifunctional metal-free catalyst by covalently bonding few layered black phosphorus nanosheets with nitrogen-doped carbon-coated multiwalled carbon nanotubes(denoted c-FBP-NC).The experimental characterizations and theoretical calculations show that the formed polarized P-N covalent bonds in c-FBP-NC can efficiently regulate electron transfer from NC to FBP and significantly promote the capture and catalysis of lithium polysulfides,thus alleviating the shuttle effect.Meanwhile,the robust 1D-2D interwoven structure with large surface area and high porosity allows strong physical confinement and fast mass transfer.Impressively,with c-FBP-NC as the sulfur host,the battery shows a high areal capacity of 7.69 mAh cm^(−2) under high sulfur loading of 8.74 mg cm^(−2) and a low electrolyte/sulfur ratio of 5.7μL mg^(−1).Moreover,the assembled pouch cell with sulfur loading of 4 mg cm^(−2) and an electrolyte/sulfur ratio of 3.5μL mg^(−1) shows good rate capability and outstanding cyclability.This work proposes an interfacial and electronic structure engineering strategy for fast and durable sulfur electrochemistry,demonstrating great potential in lithium-sulfur batteries.展开更多
文摘1.Roles of biomass and bioenergy in solar energy storage Biomass comprises plant-based material,for example,wood,microalgae,energy crops,and agro-forestry residues,as well as organic waste from industries,farms,and households,and plays a key role in solar energy capture and storage.
基金financially supported by the National Natural Science Foundation of China(52072101,51972088,U20A20122 and U1663225)the Program for Changjiang Scholars and Innovative Research Team in University(IRT_15R52)of the Chinese Ministry of Education+2 种基金the Program of Introducing Talents of Discipline to Universities-Plan 111(Grant No.B20002)from the Ministry of Science and Technology and the Ministry of Education of ChinaHubei Provincial Department of Education for the“Chutian Scholar”programsupported by the European Commission Interreg V FranceWallonie-Vlaanderen project“Depollut Air”。
文摘Owing to their high luminous efficiency and tunable emission in both red light and far-red light regions,Mn^(4+)ion-activated phosphors have appealed significant interest in photoelectric and energy conversion devices such as white light emitting diode(W-LED),plant cultivation LED,and temperature thermometer.Up to now,Mn^(4+)has been widely introduced into the lattices of various inorganic hosts for brightly redemitting phosphors.However,how to correlate the structure-activity relationship between host framework,luminescence property,and photoelectric device is urgently demanded.In this review,we thoroughly summarize the recent advances of Mn^(4+)doped phosphors.Meanwhile,several strategies like co-doping and defect passivation for improving Mn^(4+)emission are also discussed.Most importantly,the relationship between the protocols for tailoring the structures of Mn^(4+)doped phosphors,increased luminescence performance,and the targeted devices with efficient photoelectric and energy conversion efficiency is deeply correlated.Finally,the challenges and perspectives of Mn^(4+)doped phosphors for practical applications are anticipated.We cordially anticipate that this review can deliver a deep comprehension of not only Mn^(4+)luminescence mechanism but also the crystal structure tailoring strategy of phosphors,so as to spur innovative thoughts in designing advanced phosphors and deepening the applications.
基金supported by the National Natural Science Foundation of China(51976112,52206264)special Project Fund of“Taishan Scholar”of Shandong Province(tsqn202103066)Natural Science Foundation of Shandong Province(ZR2022ME109)。
文摘Biomass-to-ethylene glycol is an effective means to achieve high-value utilisation of cellulose but is hindered by low conversion efficiency and poor catalyst activity and stability.Glucose and cellobiose are derivatives of cellulose conversion to ethylene glycol,and it is found that studying the reaction process of both can help to understand the reaction mechanism of cellulose.It is desirable to develop a reusable,highly active catalyst to convert cellulose into ethylene glycol.This ideal catalyst might have one or more active sites described the conversion steps above.Here,we discuss the catalyst development of celluloseto-ethylene glycol,including tungsten,tin,lanthanide,and other transition metal catalysts,and special attention is given to the reaction mechanism and kinetics for preparing ethylene glycol from cellulose,and the economic advantages of biomass-to-ethylene glycol are briefly introduced.The insights given in this review will facilitate further development of efficient catalysts,for addressing the global energy crisis and climate change related to the use of fossil fuels.
基金supported by the National Natural Science Foundation of China (Grant Nos. 51764046 and 52160013)the Inner Mongolia Autonomous Region Postgraduate Research Innovation Project of China (Grant No. S20231165Z)the Research Program of Science and Technology at Universities of Inner Mongolia Autonomous Region of China (Grant Nos. 2023RCTD016 and 2024RCTD008)。
文摘Aerogel nanoporous materials possess high porosity, high specific surface area, and extremely low density due to their unique nanoscale network structure. Moreover, their effective thermal conductivity is very low, making them a new type of lightweight and highly efficient nanoscale super-insulating material. However, prediction of their effective thermal conductivity is challenging due to their uneven pore size distribution. To investigate the internal heat transfer mechanism of aerogel nanoporous materials, this study constructed a cross-aligned and cubic pore model(CACPM) based on the actual pore arrangement of Si O2aerogel. Based on the established CACPM, the effective thermal conductivity expression for the aerogel was derived by simultaneously considering gas-phase heat conduction, solid-phase heat conduction, and radiative heat transfer. The derived expression was then compared with available experimental data and the Wei structure model. The results indicate that, according to the model established in this study for the derived thermal conductivity formula of silica aerogel, for powdery silica aerogel under the conditions of T = 298 K, a_(2)= 0.85, D_1= 90 μm, ρ = 128 kg/m^(3), within the pressure range of 0–105Pa, the average deviation between the calculated values and experimental values is 10.51%. In the pressure range of 103–104Pa, the deviation between calculated values and experimental values is within 4%. Under these conditions, the model has certain reference value in engineering verification. This study also makes a certain contribution to the research of aerogel thermal conductivity heat transfer models and calculation formulae.
基金supported by the key project of the National Nature Science Foundation of China(51736002).
文摘Wet flue gas desulphurization technology is widely used in the industrial process for its capability of efficient pollution removal.The desulphurization control system,however,is subjected to complex reaction mechanisms and severe disturbances,which make for it difficult to achieve certain practically relevant control goals including emission and economic performances as well as system robustness.To address these challenges,a new robust control scheme based on uncertainty and disturbance estimator(UDE)and model predictive control(MPC)is proposed in this paper.The UDE is used to estimate and dynamically compensate acting disturbances,whereas MPC is deployed for optimal feedback regulation of the resultant dynamics.By viewing the system nonlinearities and unknown dynamics as disturbances,the proposed control framework allows to locally treat the considered nonlinear plant as a linear one.The obtained simulation results confirm that the utilization of UDE makes the tracking error negligibly small,even in the presence of unmodeled dynamics.In the conducted comparison study,the introduced control scheme outperforms both the standard MPC and PID(proportional-integral-derivative)control strategies in terms of transient performance and robustness.Furthermore,the results reveal that a lowpass-filter time constant has a significant effect on the robustness and the convergence range of the tracking error.
基金supported by the National Natural Science Foundation of China(51972187,22279068,52374306)the Natural Science Foundation of Shandong Province(ZR2021QE166)Qingdao New Energy Shandong Laboratory Open Project(QNESL OP202312)。
文摘The development of rechargeable magnesium(Mg) batteries is of practical significance to upgrade the electric energy storage devices due to exceptional capacity and abundant resources of Mg-metal anode.However,the reversible Mg electrochemistry suffers from unsatisfied rate capability and lifespan,mainly caused by non-uniform distribution of electrodeposits.In this work,a fresh design concept of threedimensional carbon cloths scaffolds is proposed to overcome the uncontrollable Mg growth via homogenizing electric field and improving magnesiophilicity.A microscopic smooth and nitrogen-containing defective carbonaceous layer is constructed through a facile pyrolysis of ZIF8 on carbon cloths.As revealed by finite element simulation and DFT calculation results,the smooth surface endows with uniform electric field distribution and simultaneously the nitrogen-doping species enable good magnesiophilicity of scaffolds.The fine and uniform Mg nucleus as well as the inner electrodeposit behavior are also disclosed.As a result,an exceptional cycle life of 500 cycles at 4.0 mA cm^(-2) and 4.0 mA h cm^(-2) is firstly realized to our best knowledge.Besides,the functional scaffolds can be cycled for over 2200 h at 2.0 mA cm^(-2) under a normalized capacity of 5.0 mA h cm^(-2),far exceeding previous results.This work offers an effective approach to enable the full potential of carbon cloths-based scaffolds towards metal storage for next generation battery applications.
基金supported by the Special Fund for Major State Basic Research Projects of China(2010CB732206)
文摘The paper presents an energy performance assessment of CO2 removal for crude synthetic natural gas (SNG) upgrade by Selexol absorption process. A simplified process simulation of the Selexol process concerning power requirement and separation performance was developed. The assessment indicates that less pressure difference between crude SNG and absorption pressure favors the energy performance of CO2 removal process. When both crude SNG and absorption pressures are 20 bar, CO2 removal process has the best energy performance. The optimal specific power consumption of the CO2 removal process is 566 kJ/kgCO2. The sensitivity analysis shows that the CO2 removal efficiency would significantly influence the total power consumption of the removal process, as well as higher heating value (HHV) and CO2 content in SNG. However, the specific power consumption excluding crude SNG and SNG compressions changes little with the variance of CO2 removal efficiency. If by-product CO2 is compressed for CO2 capture, the process would turn into a CO2-sink for the atmosphere. Correspondingly, an increase of 281 kJ/kgCO2 in specific power consumption is required for compressing the separated CO2.
基金Supported by the National Science Foundation of China(31500394)the Foundation and Frontier Technology Research Program of Henan Province(152300410133)the Backbone Teachers Scheme of Zhongyuan University of Technology(2014 Personnel Department of Zhongyuan University of Technology 35)
文摘As the development of city economy,Zhongdong River in Hangzhou was seriously polluted,with the worst water quality.In order to obtain the effect of water diversion and distribution from Qiantang River on the water quality of Zhongdong River,7-year continuous monitoring was conducted,which was at the fixed stations before and after the water diversion and distribution.After the water diversion project,the dissolved oxygen concentration of the river water was one to two times higher than before,and the ammonia nitrogen and total phosphorus decreased by 60%and 65%,respectively.When increased the amount of water diversion,the dissolved oxygen concentration of the river water elevated by 13%,and the ammonia nitrogen,total phosphorus and potassium permanganate index decreased by 8%,3%and 14%,respectively.The reason for the river water pollution was contributed to the combined sewer system and riverway sludge,especially during the rainfall,the dissolved oxygen concentration of Zhongdong River sharply declined by 95%,while the ammonia nitrogen and total phosphorus increased by 90%and 87%,respectively.The research results could provide theoretic basis for sustainable improvement of Zhongdong River water quality and river management department making the related regulations and policies.
基金supported by the Double Tops Joint Fund of the Yunnan Science and Technology Bureau and Yunnan University(2019FY003025)the National Natural Science Foundation of China(U2002213 and 51621001)+2 种基金the East-Land Middle-aged and Young Backbone Teacher of Yunnan University(No.C176220200)Yunnan Applied Basic Research Projects(202001BB050006,202001BB050007)the Double-First Class University Plan(C176220100042).
文摘The construction of high-efficiency and low-cost non-noble metal bifunctional electrocatalysts for water electrolysis is crucial for commercial large-scale application of hydrogen energy.Here,we report a novel strategy with erbiumdoped NiCoP nanowire arrays in situ grown on conductive nickel foam(Er-NiCoP/NF).Significantly,the developed electrode shows exceptional bifunctional catalytic activity,which only requires overpotentials of 46 and 225 mV to afford a current density of 10 mAcm^(−2) for the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OER),respectively.Density functional theory calculations reveal that the appropriate Er incorporation into the NiCoP lattice can significantly modulate the electronic structure with the d-band centers of Ni and Co atoms by shifting to lower energies with respect to the Fermi level,and optimize the Gibbs free energies of HER/OER intermediates,thereby accelerating water-splitting kinetics.When assembled as a solar-driven overall water-splitting electrolyzer,the as-prepared electrode shows a high and stable solar-to-hydrogen efficiency of 19.6%,indicating its potential for practical storage of intermittent energy.
基金the financial support from the National Key Research and Development Program of China(No.2021YFF0500802)the National Natural Science Foundation of China(No.51890904,No.52022022,and No.52278247)the Scientific Research and Innovation Plan of Jiangsu Province(KYCX21_0090)。
文摘Battery safety has attracted considerable attention worldwide due to the rapid development of wearable electronics and the steady increase in the production and use of electric vehicles.As battery failures are often associated with mechanical-thermal coupled behaviors,protective shielding materials with excellent mechanical robustness and flame-retardant properties are highly desired to mitigate thermal runaway.However,most of the thermal insulating materials are not strong enough to protect batteries from mechanical abuse,which is one of the most critical scenarios with catastrophic consequences.Here,inspired by wood,we have developed an effective approach to engineer a hierarchical nanocomposite via self-assembly of calcium silicate hydrate and polyvinyl alcohol polymer chains(referred as CSH wood).The versatile protective material CSH wood demonstrates an unprecedented combination of light weight(0.018 g cm-3),high stiffness(204 MPa in the axial direction),negative Poisson's ratio(-0.15),remarkable toughness(6.67×105 J m-3),superior thermal insulation(0.0204 W m-1 K-1 in the radial direction),and excellent fire retardancy(UL94-V0).When applied as a protective cover or a protective layer within battery packages,the tough CSH wood can resist high-impact load and block heat diffusion to block or delay the spread of fire,therefore significantly reducing the risk of property damage or bodily injuries caused by battery explosions.This work provides new pathways for fabricating advanced thermal insulating materials with large scalability and demonstrates great potential for the protection of electronic devices.
基金funded by grants from the National Natural Science Foundation of China(No.52236010,51876210)the Fundamental Research Funds for the Central Universities(No.2242022R10058)。
文摘In this work,a“cyclopentanone-vanillin”strategy was proposed for the preparation of jet fuel range cycloalkanes from lignocellulose-derived ketones and lignin-derived aldehydes via aldol condensation and hydrodeoxygenation(HDO).Ethanolamine lactate ionic liquid(LAIL)exhibited excellent catalytic activity in the aldol condensation of cyclopentanone and vanillin.Desired mono-condensation and bicondensation products were obtained with yield of 95.2%at 100℃.It is found that the synergy effects between amino group of ethanolamine and hydroxyl group of lactic acid play a key role in the aldol condensation.The condensation products were converted into cycloalkanes by HDO over 5%Pd/Nb_(2)O_(5)catalyst.The density of the obtained HDO products is 0.89 g/cm^(3)and the freezing point is lower than-60℃.These results suggest that the resulted cycloalkanes can be used as additives to improve the density and low-temperature fluidity of the jet fuels.
基金The authors would like to thank the National Natural Science Foundation of China(52176095)Anhui Provincial Natural Science Foundation(2008085J25)the Project of support program for outstanding young people in Colleges and Universities(gxyqZD201830)for their financial support of this study.
文摘The laminar combustion characteristics of CH_(4)/air premixed flames with CO_(2) addition are systemically studied.Experimental measurements and numerical simulations of the laminar burning velocity(LBV)are performed in CH_(4)/CO_(2)/Air flames with various CO_(2) doping ratio under equivalence ratios of 1.0–1.4.GRI 3.0 mech and Aramco mech are employed for predicting LBV,adiabatic flame temperature(AFT),important intermediate radicals(CH_(3),H,OH,O)and NO_(x) emissions(NO,NO_(2),N2O),as well as the sensitivity analysis is also conducted.The detail analysis of experiment and simulation reveals that as the CO_(2) addition increases from 0%to 40%,the LBVs and AFTs decrease monotonously.Under the same CO_(2) doping ratio,the LBVs and AFTs increase first and then decrease with the increase of equivalence ratio,and the maximum of LBV is reached at equivalence ratio of 1.05.The mole fraction tendency of important intermediates and NO_(x) with equivalence ratio and CO_(2) doping ratio are similar to the LBVs and AFTs.Reaction H+O_(2)⇔O+OH is found to be responsible for the promotion of the generation of important intermediates and NO_(x) under the equivalence ratios and CO_(2) addition through sensitivity analysis.The sensitivity coefficients of elementary reactions that the increasing of CO_(2) doping ratio promotes or inhibits formation of intermediate radicals and NO_(x) decreases.
基金supported by a Research Matching Grant Scheme(PJ9229008)by the government of Hong Kong Special Administrative Region。
文摘Cu-Li battery with Cu metal cathode and Li metal anode is a candidate for next-generation energy storage system.While self-discharge of the battery can be suppressed with an anion exchange membrane,the voltage polarization depends strongly on the electrolyte.Specifically,when an electrolyte with 3 M LiTFSI(lithium bis(trifluoromethanesulfonyl)imide)in dimethyl carbonate(DMC)is used,overpotential increases with cycling.In this work,we reveal why the voltage polarization changes,and reduce and stabilize it by replacing DMC solvent with a mixed solvent composed of dimethoxyethane(DME)and propylene carbonate(PC).The new electrolyte has higher ionic conductivity and stable solvation structure with more free TFSI-anions upon cycling,which also facilitates uniform plating of metal ions on the metal electrodes.These characteristics enable a stable Cu-Li battery with minimal change in overpotential for more than 1500 cycles at a current density of 2 m A cm^(-2).
基金This work was supported financially by the National Key R&D Program of China(2018YFB1501500)National Natural Science Foundation of China(51976225).
文摘Since the utilization of abundant biomass to develop advanced materials has become an utmost priority in recent years,we developed two sustainable routes(i.e.,the impregnation method and the one-pot synthesis)to prepare the hydrochar-supported catalysts and tested its catalytic performance on the reductive amination.Several techniques,such as TEM,XRD and XPS,were adopted to characterize the structural and catalytic features of samples.Results indicated that the impregnation method favors the formation of outer-sphere surface complexes with porous structure as well as well-distributed metallic nanoparticles,while the one-pot synthesis tends to form the inner-sphere surface complexes with relatively smooth appearance and amorphous metals.This difference explains the better activity of catalysts prepared by the impregnation method which can selectively convert benzaldehyde to benzylamine with an excellent yield of 93.7%under the optimal reaction conditions;in contrast,the catalyst prepared by the one-pot synthesis only exhibits a low selectivity near to zero.Furthermore,the gram-scale test catalyzed by the same catalysts exhibits a similar yield of benzylamine in comparison to its smaller scale,which is comparable to the previously reported heterogeneous noble-based catalysts.More surprisingly,the prepared catalysts can be expediently recycled by a magnetic bar and remain the satisfying catalytic activity after reusing up to five times.In conclusion,these developed catalysts enable the synthesis of functional amines with excellent selectivity and carbon balance,proving cost-effective and sustainable access to the wide application of reductive amination.
基金Financial support was provided by the Guangdong College Students’Innovative Project(202110580014)the Guangdong “Climbing”Program for Research Items(pdjh2021b0544)。
文摘The next-generation energy storage systems such as fuel cells,metal-air batteries,and alkali metal(Li,Na)-chalcogen(S,Se)batteries have received increasing attention owing to their high energy density and low cost.However,one of the main obstacles of these systems is the poor reaction kinetics in the involved chemical reactions.Therefore,it is essential to incorporate suitable and efficient catalysts into the cell.These years,single-atom catalysts(SACs)are emerging as a frontier in catalysis due to their maximum atom efficiency and unique reaction selectivity.For SACs fabrication,metal-organic frameworks(MOFs)have been confirmed as promising templates or precursors due to their high metal loadings,structural adjustability,porosity,and tailorable catalytic site.In this review,we summarize effective strategies for fabricating SACs by MOFs with corresponding advanced characterization techniques and illustrate the key role of MOFs-based SACs in these batteries by explaining their reaction mechanisms and challenges.Finally,current applications,prospects,and opportunities for MOFs-based SACs in energy storage systems are discussed.
基金supported by National Natural Science Foundation of China(Grant No.52100084)Shenzhen Natural Science Fund(the Stable Support Plan Program GXWD20201230155427003-20200824094017001).
文摘Air-stable layered structured cathodes with high voltage and good cycling stability are highly desired for the practical application of Na-ion batteries.Herein,we report a P2-Na_(2/3)Ni_(2/3)Te_(1/3)O_(2) cathode that is stable in ambient air with an average operating voltage of~3.8 V,demonstrating excellent cycling stability with a capacity retention of more than 92.7%after 500 cycles at 20 mA g^(-1) and good rate capability with 91.9%capacity utilization at 500 mA g^(-1) with respect to capacity at 5 mA g^(-1) between 2.0 and 4.0 V.When the upper cutoff voltage is increased to 4.4 V,P2-Na_(2/3)Ni_(2/3)Te_(1/3)O_(2) delivers a reversible capacity of 71.9 mAh g^(-1) and retains 91.8%of the capacity after 100 cycles at 20 mA g^(-1).The charge compensation during charge/discharge is mainly due to the redox couple of Ni^(2+)/Ni^(3+)in the host with a small amount of contribution from oxygen.The stable structure of the material without phase transformation and with small volume change during charge-discharge allows it to give excellent cycle performance especially when the upper cutoff voltage is not higher than 4.2 V.
基金jointly supported by the National Natural Science Foundation of China (Grant Nos. 42120104001, 41805042)the Science and Technology Program of Guangzhou, China (Grant No. 202102020939)+1 种基金the Fundamental Research Funds for the Central University, Sun Yat-Sen University (Grant No. 22qntd2202)a project of the Center for Ocean Research in Hong Kong and Macao (CORE)
文摘During boreal winter,the invasion of cold air can lead to remarkable temperature drops in East Asia which can result in serious socioeconomic impacts.Here,we find that the intensity of strong synoptic cold days in the East China Sea and Indochina Peninsula are increasing.The enhanced synoptic cold days in these two regions are attributed to surface warming over the South China Sea and Philippine Sea(SCSPS).The oceanic forcing of the SCSPS on the synoptic cold days in the two regions is verified by numerical simulation.The warming of the SCSPS enhances the baroclinicity,which intensifies meridional wind and cold advection on synoptic timescales.This leads to a more extended region that is subject to the influence of cold invasion.
基金supported by the National Natural Science Foundation of China(22179070,U1932220)the Natural Science Foundation of Jiangsu Province(BK20220073)the Fundamental Research Funds for the Central Universities(RF1028623157)。
文摘Safe batteries are the basis for next-generation application scenarios such as portable energy storage devices and electric vehicles,which are crucial to achieving carbon neutralization.Electrolytes,separators,and electrodes as main components of lithium batteries strongly affect the occurrence of safety accidents.Responsive materials,which can respond to external stimuli or environmental change,have triggered extensive attentions recently,holding great promise in facilitating safe and smart batteries.This review thoroughly discusses recent advances regarding the construction of high-safety lithium batteries based on internal thermal-responsive strategies,together with the corresponding changes in electrochemical performance under external stimulus.Furthermore,the existing challenges and outlook for the design of safe batteries are presented,creating valuable insights and proposing directions for the practical implementation of safe lithium batteries.
基金Jiangsu Provincial Department of Science and Technology,Grant/Award Number:BK20201190Fundamental Research Funds for“Young Talent Support Plan”of Xi'an Jiaotong University,Grant/Award Number:HG6J003+1 种基金“1000-Plan program”of Shaanxi Province and the Velux Foundations through the research center V-Sustain,Grant/Award Number:9455National Key R&D Program of China,。
文摘The use of lithium-sulfur batteries under high sulfur loading and low electrolyte concentrations is severely restricted by the detrimental shuttling behavior of polysulfides and the sluggish kinetics in redox processes.Two-dimensional(2D)few layered black phosphorus with fully exposed atoms and high sulfur affinity can be potential lithium-sulfur battery electrocatalysts,which,however,have limitations of restricted catalytic activity and poor electrochemical/chemical stability.To resolve these issues,we developed a multifunctional metal-free catalyst by covalently bonding few layered black phosphorus nanosheets with nitrogen-doped carbon-coated multiwalled carbon nanotubes(denoted c-FBP-NC).The experimental characterizations and theoretical calculations show that the formed polarized P-N covalent bonds in c-FBP-NC can efficiently regulate electron transfer from NC to FBP and significantly promote the capture and catalysis of lithium polysulfides,thus alleviating the shuttle effect.Meanwhile,the robust 1D-2D interwoven structure with large surface area and high porosity allows strong physical confinement and fast mass transfer.Impressively,with c-FBP-NC as the sulfur host,the battery shows a high areal capacity of 7.69 mAh cm^(−2) under high sulfur loading of 8.74 mg cm^(−2) and a low electrolyte/sulfur ratio of 5.7μL mg^(−1).Moreover,the assembled pouch cell with sulfur loading of 4 mg cm^(−2) and an electrolyte/sulfur ratio of 3.5μL mg^(−1) shows good rate capability and outstanding cyclability.This work proposes an interfacial and electronic structure engineering strategy for fast and durable sulfur electrochemistry,demonstrating great potential in lithium-sulfur batteries.