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
Combining single atoms with clusters or nanoparticles is an emerging tactic to design efficient electrocatalysts.Both synergy effect and high atomic utilization of active sites in the composite catalysts result in enh...Combining single atoms with clusters or nanoparticles is an emerging tactic to design efficient electrocatalysts.Both synergy effect and high atomic utilization of active sites in the composite catalysts result in enhanced electrocatalytic performance,simultaneously provide a radical analysis of the interrelationship between structure and activity.In this review,the recent advances of single-atomic site catalysts coupled with clusters or nanoparticles are emphasized.Firstly,the synthetic strategies,characterization,dynamics and types of single atoms coupled with clusters/nanoparticles are introduced,and then the key factors controlling the structure of the composite catalysts are discussed.Next,several clean energy catalytic reactions performed over the synergistic composite catalysts are illustrated.Eventually,the encountering challenges and recommendations for the future advancement of synergistic structure in energy-transformation electrocatalysis are outlined.展开更多
Mesoporous CeMnOx composite oxides catalysts were prepared by surfactant-assisted co-precipitation method and used for the catalytic oxidation of toluene.The effect of different cerium precursors[Ce(NO3)3 and(NH4)2 Ce...Mesoporous CeMnOx composite oxides catalysts were prepared by surfactant-assisted co-precipitation method and used for the catalytic oxidation of toluene.The effect of different cerium precursors[Ce(NO3)3 and(NH4)2 Ce(NO3)6] on catalyst structure,surface properties and toluene combustion activities of mesoporous CeMnOx catalysts were investigated.The Ce(Ⅲ)MnOx catalyst prepared from Ce(NO3)3 precursor shows higher catalytic activity,with a 90% conversion temperature of 240℃,which is better than the Ce(Ⅳ)MnOx catalyst derived from[(NH4)2 Ce(NO3)6] precursor.On the basis of characterizations,it reveals that abundant surface content of Mn4+,better redox behavior and larger concentration of surface active oxygen species are responsible for the excellent catalytic performance.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(22279036)the Innovation Talent Recruitment Base of New Energy Chemistry Device(B21003)the Fundamental Research Funds for the Central Universities(no.2019kfyRCPY100).
文摘Combining single atoms with clusters or nanoparticles is an emerging tactic to design efficient electrocatalysts.Both synergy effect and high atomic utilization of active sites in the composite catalysts result in enhanced electrocatalytic performance,simultaneously provide a radical analysis of the interrelationship between structure and activity.In this review,the recent advances of single-atomic site catalysts coupled with clusters or nanoparticles are emphasized.Firstly,the synthetic strategies,characterization,dynamics and types of single atoms coupled with clusters/nanoparticles are introduced,and then the key factors controlling the structure of the composite catalysts are discussed.Next,several clean energy catalytic reactions performed over the synergistic composite catalysts are illustrated.Eventually,the encountering challenges and recommendations for the future advancement of synergistic structure in energy-transformation electrocatalysis are outlined.
基金Project supported by the National Natural Science Foundation of China(21503184)the Natural Science Foundation of Jiangsu ProvinceGeneral Program(BK20171273)+1 种基金the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(18KJA610004)the Opening Project of the Jiangsu Key Laboratory for Environment Functional Materials(SJHG1806)
文摘Mesoporous CeMnOx composite oxides catalysts were prepared by surfactant-assisted co-precipitation method and used for the catalytic oxidation of toluene.The effect of different cerium precursors[Ce(NO3)3 and(NH4)2 Ce(NO3)6] on catalyst structure,surface properties and toluene combustion activities of mesoporous CeMnOx catalysts were investigated.The Ce(Ⅲ)MnOx catalyst prepared from Ce(NO3)3 precursor shows higher catalytic activity,with a 90% conversion temperature of 240℃,which is better than the Ce(Ⅳ)MnOx catalyst derived from[(NH4)2 Ce(NO3)6] precursor.On the basis of characterizations,it reveals that abundant surface content of Mn4+,better redox behavior and larger concentration of surface active oxygen species are responsible for the excellent catalytic performance.
