In this work,we open an avenue toward rational design of potential efficient catalysts for sustainable ammonia synthesis through composition engineering strategy by exploiting the synergistic effects among the active ...In this work,we open an avenue toward rational design of potential efficient catalysts for sustainable ammonia synthesis through composition engineering strategy by exploiting the synergistic effects among the active sites as exemplified by diatomic metals anchored graphdiyne via the combination of hierarchical high-throughput screening,first-principles calculations,and molecular dynamics simulations.Totally 43 highly efficient catalysts feature ultralow onset potentials(|U_(onset)|≤0.40 V)with Rh-Hf and Rh-Ta showing negligible onset potentials of 0 and-0.04 V,respectively.Extremely high catalytic activities of Rh-Hf and Rh-Ta can be ascribed to the synergistic effects.When forming heteronuclears,the combinations of relatively weak(such as Rh)and relatively strong(such as Hf or Ta)components usually lead to the optimal strengths of adsorption Gibbs free energies of reaction intermediates.The origin can be ascribed to the mediate d-band centers of Rh-Hf and Rh-Ta,which lead to the optimal adsorption strengths of intermediates,thereby bringing the high catalytic activities.Our work provides a new and general strategy toward the architecture of highly efficient catalysts not only for electrocatalytic nitrogen reduction reaction(eNRR)but also for other important reactions.We expect that our work will boost both experimental and theoretical efforts in this direction.展开更多
As an ideal solution to energy and environment issues,conversion of sunlight into solar fuels by photocatalytic water splitting and greenhouse gas(CO_2)reduction has attracted keen research interest of multi-field sci...As an ideal solution to energy and environment issues,conversion of sunlight into solar fuels by photocatalytic water splitting and greenhouse gas(CO_2)reduction has attracted keen research interest of multi-field scientists.In the past four decades,a large number of semiconductor photocatalysts have been展开更多
While most of the present medical implants are nonbiodegradable,biodegradable materials are thought to replace many nonbiodegradable ones in the future,which is dependent on development of the corresponding core techn...While most of the present medical implants are nonbiodegradable,biodegradable materials are thought to replace many nonbiodegradable ones in the future,which is dependent on development of the corresponding core techniques of biomaterials[1-4].Much progress has been made in the field of biodegradable materials during the last decade[5-7].展开更多
基金support from the National Natural Science Foundation of China(22073033,21873032,21673087,21903032)startup fund(2006013118 and 3004013105)from Huazhong University of Science and Technology+1 种基金the Fundamental Research Funds for the Central Universities(2019kfyRCPY116)the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)
文摘In this work,we open an avenue toward rational design of potential efficient catalysts for sustainable ammonia synthesis through composition engineering strategy by exploiting the synergistic effects among the active sites as exemplified by diatomic metals anchored graphdiyne via the combination of hierarchical high-throughput screening,first-principles calculations,and molecular dynamics simulations.Totally 43 highly efficient catalysts feature ultralow onset potentials(|U_(onset)|≤0.40 V)with Rh-Hf and Rh-Ta showing negligible onset potentials of 0 and-0.04 V,respectively.Extremely high catalytic activities of Rh-Hf and Rh-Ta can be ascribed to the synergistic effects.When forming heteronuclears,the combinations of relatively weak(such as Rh)and relatively strong(such as Hf or Ta)components usually lead to the optimal strengths of adsorption Gibbs free energies of reaction intermediates.The origin can be ascribed to the mediate d-band centers of Rh-Hf and Rh-Ta,which lead to the optimal adsorption strengths of intermediates,thereby bringing the high catalytic activities.Our work provides a new and general strategy toward the architecture of highly efficient catalysts not only for electrocatalytic nitrogen reduction reaction(eNRR)but also for other important reactions.We expect that our work will boost both experimental and theoretical efforts in this direction.
基金financially supported by the National Natural Science Foundation of China (U1305242 and 21673043)
文摘As an ideal solution to energy and environment issues,conversion of sunlight into solar fuels by photocatalytic water splitting and greenhouse gas(CO_2)reduction has attracted keen research interest of multi-field scientists.In the past four decades,a large number of semiconductor photocatalysts have been
文摘While most of the present medical implants are nonbiodegradable,biodegradable materials are thought to replace many nonbiodegradable ones in the future,which is dependent on development of the corresponding core techniques of biomaterials[1-4].Much progress has been made in the field of biodegradable materials during the last decade[5-7].