Tuning the coordination atoms of central metal is an effective means to improve the electrocatalytic activity of atomic catalysts.Herein,iridium(Ir) is proposed to be asymmetrically anchored by sp-N and pyridinic N of...Tuning the coordination atoms of central metal is an effective means to improve the electrocatalytic activity of atomic catalysts.Herein,iridium(Ir) is proposed to be asymmetrically anchored by sp-N and pyridinic N of hydrogen-substituted graphdiyne(HsGDY),and coordinated with OH as an Ir atomic catalyst(Ir_(1)-N-HsGDY).The electron structures,especially the d-band center of Ir atom,are optimized by these specific coordination atoms.Thus,the as-synthesized Ir_(1)-N-HsGDY exhibits excellent electrocatalytic performances for oxygen reduction and hydrogen evolution reactions in both acidic and alkaline media.Benefiting from the unique structure of HsGDY,IrN_(2)(OH)_(3) has been developed and demonstrated to act as the active site in these electrochemical reactions.All those indicate the fresh role of the sp-N in graphdiyne in producing a new anchor way and contributing to promote the electrocatalytic activity,showing a new strategy to design novel electrochemical catalysts.展开更多
The figure of merit is of crucial importance in materials design to search for candidates with optimal functionality.In the field of photovoltaics,the bandgap(E_g)is a well-recognized figure of merit for screening sol...The figure of merit is of crucial importance in materials design to search for candidates with optimal functionality.In the field of photovoltaics,the bandgap(E_g)is a well-recognized figure of merit for screening solar cell absorbers subject to the Shockley-Queisser limit.In this paper,the bandgap as the figure of merit is challenged since an ideal solar cell absorber requires multiple criteria such as stability,optical absorption,and carrier lifetime.Multiple criteria make the quantitative description of material candidates difficult and computationally time-consuming.Taking halide perovskites as an example,we combine thermodynamic stability(ΔHd)and Eginto a unified figure of merit and use Bayesian optimization(BO)to accelerate materials screening.We have found that,in comparison to an exhaustive search via multiple parameters,BO based on the unified figure of merit can screen optimal candidates(E_g,PBEbetween 0.6–1.2 eV,ΔHd>-29 meV per atom)more efficiently.Therefore,the proposed method opens a viable route for the search of optimal solar cell absorbers from a large amount of material candidates with less computational cost.展开更多
基金supported by the National Natural Science Foundation of China(22172090,21790051)the National Key Research and Development Project of China(2022YFA1204500,2022YFA1204501)+2 种基金the Natural Science Foundation of Shan-dong Province(ZR2021MB015)the Open Funds of the State Key Laboratory of Electroanalytical Chemistry(SKLEAC202202)the Young Scholars Program of Shandong University。
文摘Tuning the coordination atoms of central metal is an effective means to improve the electrocatalytic activity of atomic catalysts.Herein,iridium(Ir) is proposed to be asymmetrically anchored by sp-N and pyridinic N of hydrogen-substituted graphdiyne(HsGDY),and coordinated with OH as an Ir atomic catalyst(Ir_(1)-N-HsGDY).The electron structures,especially the d-band center of Ir atom,are optimized by these specific coordination atoms.Thus,the as-synthesized Ir_(1)-N-HsGDY exhibits excellent electrocatalytic performances for oxygen reduction and hydrogen evolution reactions in both acidic and alkaline media.Benefiting from the unique structure of HsGDY,IrN_(2)(OH)_(3) has been developed and demonstrated to act as the active site in these electrochemical reactions.All those indicate the fresh role of the sp-N in graphdiyne in producing a new anchor way and contributing to promote the electrocatalytic activity,showing a new strategy to design novel electrochemical catalysts.
基金Yin WJ acknowledges funding support from the National Key Research and Development Program of China(2016YFB0700700)the National Natural Science Foundation of China(11974257,11674237 and 51602211)+1 种基金the Natural Science Foundation of Jiangsu Province of China(BK20160299)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD).The theoretical work was carried out at the National Supercomputer Center in Tianjin and the calculations were performed on TianHe-l(A).
文摘The figure of merit is of crucial importance in materials design to search for candidates with optimal functionality.In the field of photovoltaics,the bandgap(E_g)is a well-recognized figure of merit for screening solar cell absorbers subject to the Shockley-Queisser limit.In this paper,the bandgap as the figure of merit is challenged since an ideal solar cell absorber requires multiple criteria such as stability,optical absorption,and carrier lifetime.Multiple criteria make the quantitative description of material candidates difficult and computationally time-consuming.Taking halide perovskites as an example,we combine thermodynamic stability(ΔHd)and Eginto a unified figure of merit and use Bayesian optimization(BO)to accelerate materials screening.We have found that,in comparison to an exhaustive search via multiple parameters,BO based on the unified figure of merit can screen optimal candidates(E_g,PBEbetween 0.6–1.2 eV,ΔHd>-29 meV per atom)more efficiently.Therefore,the proposed method opens a viable route for the search of optimal solar cell absorbers from a large amount of material candidates with less computational cost.
