Lithium-sulfur(Li-S)batteries are notable for their high theoretical energy density,but the‘shuttle effect’and the limited conversion kinetics of Li-S species can downgrade their actual performance.An essential stra...Lithium-sulfur(Li-S)batteries are notable for their high theoretical energy density,but the‘shuttle effect’and the limited conversion kinetics of Li-S species can downgrade their actual performance.An essential strategy is to design anchoring materials(AMs)to appropriately adsorb Li-S species.Herein,we propose a new three-procedure protocol,named InfoAd(Informative Adsorption)to evaluate the anchoring of Li_(2)S on two-dimensional(2D)materials and disclose the underlying importance of material features by combining high-throughput calculation workflow and machine learning(ML).In this paradigm,we calculate the anchoring of Li_(2)S on 12552D A_(x)B_(y)(B in the VIA/VIIA group)materials and pick out 44(un)reported nontoxic 2D binary A_(x)B_(y)AMs,in which the importance of the geometric features on the anchoring effect is revealed by ML for the first time.We develop a new Infograph model for crystals to accurately predict whether a material has a moderate binding with Li_(2)S and extend it to all 2D materials.Our InfoAd protocol elucidates the underlying structure-property relationship of Li_(2)S adsorption on 2D materials and provides a general research framework of adsorption-related materials for catalysis and energy/substance storage.展开更多
Providing efficient charge transfer through the interface between the semiconductor and co-catalyst is greatly desired in photoelectrocatalytic (PEC) energy conversion.Herein,we excogitate a novel and facile means,via...Providing efficient charge transfer through the interface between the semiconductor and co-catalyst is greatly desired in photoelectrocatalytic (PEC) energy conversion.Herein,we excogitate a novel and facile means,via electrochemical activation,to successfully load the amorphous CoOOH layer architecture onto the surface of TiO_(2).Intriguingly,the as-obtained 6%CoOOH-TiO_(2)photoelectrode manifests optimal PEC performance with a high photocurrent density of 1.3 mA/cm~2,3.5 times higher than that of pristine TiO_(2).Electrochemical impedance spectroscopy (EIS),Tafel analysis and cyclic voltammetry (CV) methods show that the carrier transfer barrier within the electrode and the transition of Co^(3+)OOH to Co^(4+)OOH have the dominating effects on the PEC performance.Theoretical calculation reveals that the interface between the CoOOH and TiO_(2)improves the homogeneity of effective d-orbital electronic-transfer ability among Co sites.This research sheds light on the water oxidation reaction and the design of more favorable PEC cocatalysts.展开更多
The design of electrocatalysts with enhanced adsorption and activation of nitrogen(N2)is critical for boosting the electrochemical N2reduction(ENR).Herein,we developed an efficient strategy to facilitate N2 adsorption...The design of electrocatalysts with enhanced adsorption and activation of nitrogen(N2)is critical for boosting the electrochemical N2reduction(ENR).Herein,we developed an efficient strategy to facilitate N2 adsorption and activation for N2 electroreduction into ammonia(NH3)by vacancy engineering of core@shell structured Au@Sn O2 nanoparticles(NPs).We found that the ultrathin amorphous SnO2 shell with enriched oxygen vacancies was conducive to adsorb N2as well as promoted the N2 activation,meanwhile the metallic Au core ensured the good electrical conductivity for accelerating electrons transport during the electrochemical N2 reduction reaction,synergistically boosting the N2 electroreduction catalysis.As confirmed by the15N-labeling and controlled experiments,the core@shell Au@amorphous SnO2 NPs with abundant oxygen vacancies show the best performance for N2 electroreduction with the NH3 yield rate of 21.9 lg h-1mg-1catand faradaic efficiency of 15.2%at-10.2 VRHE,which surpass the Au@crystalline SnO2 NPs,individual Au NPs and all reported Au-based catalysts for ENR.展开更多
Among all CO2 electroreduction products,methane(CH4)and ethylene(C_(2)H_(4))are two typical and valuable hydrocarbon products which are formed in two different pathways:hydrogenation and dimerization reactions of the ...Among all CO2 electroreduction products,methane(CH4)and ethylene(C_(2)H_(4))are two typical and valuable hydrocarbon products which are formed in two different pathways:hydrogenation and dimerization reactions of the same CO intermediate.Theoretical studies show that the adsorption configurations of CO intermediate determine the reaction pathways towards CH4/C_(2)H_(4).However,it is challenging to experimentally control the CO adsorption configurations at the catalyst surface,and thus the hydrocarbon selectivity is still limited.Herein,we seek to synthesize two well-defined copper nanocatalysts with controllable surface structures.The two model catalysts exhibit a high hydrocarbon selectivity toward either CH4(83%)or C_(2)H_(4)(93%)under identical reduction conditions.Scanning transmission electron microscopy and X-ray absorption spectroscopy characterizations reveal the low-coordination Cu^(0)sites and local Cu^(0)/Cu^(+)sites of the two catalysts,respectively.CO-temperature programed desorption,in-situ attenuated total reflection Fourier transform infrared spectroscopy and density functional theory studies unveil that the bridge-adsorbed CO(CO_(B))on the low-coordination Cu^(0)sites is apt to be hydrogenated to CH4,whereas the bridge-adsorbed CO plus linear-adsorbed CO(CO_(B)+CO_(L))on the local Cu^(0)/Cu^(+)sites are apt to be coupled to C_(2)H_(4).Our findings pave a new way to design catalysts with controllable CO adsorption configurations for high hydrocarbon product selectivity.展开更多
基金supported by National key research and development program of China(2022YFA1503101)National Natural Science Foundation of China(22173067,22203058)+4 种基金Science and Technology Project of Jiangsu Province(BK20200873,BZ2020011)the Science and Technology Development Fund,Macao SAR(0052/2021/A)Collaborative Innovation Center of Suzhou Nano Science&Technology,the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)the 111 ProjectJoint International Research Laboratory of Carbon-Based Functional Materials and Devices。
文摘Lithium-sulfur(Li-S)batteries are notable for their high theoretical energy density,but the‘shuttle effect’and the limited conversion kinetics of Li-S species can downgrade their actual performance.An essential strategy is to design anchoring materials(AMs)to appropriately adsorb Li-S species.Herein,we propose a new three-procedure protocol,named InfoAd(Informative Adsorption)to evaluate the anchoring of Li_(2)S on two-dimensional(2D)materials and disclose the underlying importance of material features by combining high-throughput calculation workflow and machine learning(ML).In this paradigm,we calculate the anchoring of Li_(2)S on 12552D A_(x)B_(y)(B in the VIA/VIIA group)materials and pick out 44(un)reported nontoxic 2D binary A_(x)B_(y)AMs,in which the importance of the geometric features on the anchoring effect is revealed by ML for the first time.We develop a new Infograph model for crystals to accurately predict whether a material has a moderate binding with Li_(2)S and extend it to all 2D materials.Our InfoAd protocol elucidates the underlying structure-property relationship of Li_(2)S adsorption on 2D materials and provides a general research framework of adsorption-related materials for catalysis and energy/substance storage.
基金support from the National Key Research Program of China (2017YFA0204800, 2016YFA0202403)the Natural Science Foundation of China (No. 21603136)+3 种基金the Changjiang Scholar and Innovative Research Team (IRT_14R33)the Fundamental Research Funds for the Central Universities (GK202003042)The 111 Project (B14041)the Chinese National 1000-Talent-Plan program are also acknowledged。
文摘Providing efficient charge transfer through the interface between the semiconductor and co-catalyst is greatly desired in photoelectrocatalytic (PEC) energy conversion.Herein,we excogitate a novel and facile means,via electrochemical activation,to successfully load the amorphous CoOOH layer architecture onto the surface of TiO_(2).Intriguingly,the as-obtained 6%CoOOH-TiO_(2)photoelectrode manifests optimal PEC performance with a high photocurrent density of 1.3 mA/cm~2,3.5 times higher than that of pristine TiO_(2).Electrochemical impedance spectroscopy (EIS),Tafel analysis and cyclic voltammetry (CV) methods show that the carrier transfer barrier within the electrode and the transition of Co^(3+)OOH to Co^(4+)OOH have the dominating effects on the PEC performance.Theoretical calculation reveals that the interface between the CoOOH and TiO_(2)improves the homogeneity of effective d-orbital electronic-transfer ability among Co sites.This research sheds light on the water oxidation reaction and the design of more favorable PEC cocatalysts.
基金supported by the National Key Research Program of China (2022YFA1503101)the National Natural Science Foundation of China (22173067)+3 种基金the Science and Technology Development Fund, Macao SAR (FDCT, 0024/2022/ITP)the Collaborative Innovation Center of Suzhou Nano Science & Technology, Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)the 111 Projectthe Joint International Research Laboratory of Carbon-Based Functional Materials and Devices。
基金supported by the National Key R&D Program of China(2016YFA0204100 and 2017YFA0208200)the National Natural Science Foundation of China(21571135)+5 种基金Young Thousand Talented ProgramNatural Science Foundation of Jiangsu Higher Education Institutions(17KJB150032)the Project of Scientific and Technologic Infrastructure of Suzhou(SZS201708)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX19_1896)the Start-Up Supports from Soochow University.
文摘The design of electrocatalysts with enhanced adsorption and activation of nitrogen(N2)is critical for boosting the electrochemical N2reduction(ENR).Herein,we developed an efficient strategy to facilitate N2 adsorption and activation for N2 electroreduction into ammonia(NH3)by vacancy engineering of core@shell structured Au@Sn O2 nanoparticles(NPs).We found that the ultrathin amorphous SnO2 shell with enriched oxygen vacancies was conducive to adsorb N2as well as promoted the N2 activation,meanwhile the metallic Au core ensured the good electrical conductivity for accelerating electrons transport during the electrochemical N2 reduction reaction,synergistically boosting the N2 electroreduction catalysis.As confirmed by the15N-labeling and controlled experiments,the core@shell Au@amorphous SnO2 NPs with abundant oxygen vacancies show the best performance for N2 electroreduction with the NH3 yield rate of 21.9 lg h-1mg-1catand faradaic efficiency of 15.2%at-10.2 VRHE,which surpass the Au@crystalline SnO2 NPs,individual Au NPs and all reported Au-based catalysts for ENR.
基金supported by the National Natural Science Foundation of China (21875042)Shanghai Science and Technology Committee (18QA1400800)+1 种基金the Program of Eastern Scholar at Shanghai Institutions and Yanchang Petroleum Groupsupported by the Frontier Research Center for Materials Structure, School of Materials Science and Engineering of Shanghai Jiao Tong University
文摘Among all CO2 electroreduction products,methane(CH4)and ethylene(C_(2)H_(4))are two typical and valuable hydrocarbon products which are formed in two different pathways:hydrogenation and dimerization reactions of the same CO intermediate.Theoretical studies show that the adsorption configurations of CO intermediate determine the reaction pathways towards CH4/C_(2)H_(4).However,it is challenging to experimentally control the CO adsorption configurations at the catalyst surface,and thus the hydrocarbon selectivity is still limited.Herein,we seek to synthesize two well-defined copper nanocatalysts with controllable surface structures.The two model catalysts exhibit a high hydrocarbon selectivity toward either CH4(83%)or C_(2)H_(4)(93%)under identical reduction conditions.Scanning transmission electron microscopy and X-ray absorption spectroscopy characterizations reveal the low-coordination Cu^(0)sites and local Cu^(0)/Cu^(+)sites of the two catalysts,respectively.CO-temperature programed desorption,in-situ attenuated total reflection Fourier transform infrared spectroscopy and density functional theory studies unveil that the bridge-adsorbed CO(CO_(B))on the low-coordination Cu^(0)sites is apt to be hydrogenated to CH4,whereas the bridge-adsorbed CO plus linear-adsorbed CO(CO_(B)+CO_(L))on the local Cu^(0)/Cu^(+)sites are apt to be coupled to C_(2)H_(4).Our findings pave a new way to design catalysts with controllable CO adsorption configurations for high hydrocarbon product selectivity.
