Electrochemical reduction of water to hydrogen holds great promise for clean energy,while its widespread application relies on the development of efficient catalysts with large surface area,abundant exposed active sit...Electrochemical reduction of water to hydrogen holds great promise for clean energy,while its widespread application relies on the development of efficient catalysts with large surface area,abundant exposed active sites and superior electron conductivity.Herein,we report a facile strategy to configure an electrocatalyst composed of cobalt phosphide and rhodium uniformly anchored on reduced graphene oxide for hydrogen generation.The hybrids effectively integrate the exposed active sites,electron conductivity and synergistic effect of the catalyst.Electrochemical tests exhibit that the catalyst shows superior hydrogen evolution reaction catalytic activity and stability,with a small Tafel slope of 43 m V dec-1.Overpotentials as low as 29 and 72 mV are required to achieve current densities of 2 and 10 mA cm-2in 0.5M H2SO4,respectively.The hybrid constitution with highly active sites on conductive substrate is a new strategy to synthesize extremely efficient electrocatalysts.Especially,the efficient synergistic effect among cobalt phosphide,rhodium and reduced graphene oxide provides a novel approach for configuring electrocatalysts with high electron efficiency.展开更多
Over the past decades, the energy and concomitant environment issues, such as energy shortage, air pollution and global warming, have been becoming increasingly striking world-wide challenges [1,2]. Such a dilemma in ...Over the past decades, the energy and concomitant environment issues, such as energy shortage, air pollution and global warming, have been becoming increasingly striking world-wide challenges [1,2]. Such a dilemma in turn appeals to the development and employment of clean and renewable energy.展开更多
Simultaneous achievement of constructing mesopores and eliminating anatase is a long-term pursuit for enhancing the catalytic performance of TS-1.Here,we developed an aromatic compounds-mediated synthesis method to pr...Simultaneous achievement of constructing mesopores and eliminating anatase is a long-term pursuit for enhancing the catalytic performance of TS-1.Here,we developed an aromatic compounds-mediated synthesis method to prepare anatase-free and hierarchical TS-1 for olefin epoxidation.A series of hierarchical TS-1 zeolites were prepared by introducing aromatic compounds containing different functional groups via the crystallization process.The formation of intercrystalline mesopores and insertion of titanium into framework were facilitated at different extent.The synergistic coordination of carboxyl and hydroxyl in aromatic compounds with Ti(OH)4 realizes the uniform distribution of titanium species and eliminates the generation of anatase.Noteworthily,eight machine learning models were trained to reveal the mechanism of additive functional groups and preparation conditions on anatase formation and microstructure optimization.The prediction accuracy of most models can reach more than 80%.Benefiting from the larger mesopore volumes(0.37 cm3⋅g−1)and higher content of framework Ti species,TS-DHBDC-48h samples exhibit a higher catalytic performance than other zeolites,giving 1-hexene conversion of 49.3%and 1,2-epoxyhenane selectivity of 99.9%.The paper provides a facile aromatic compounds-mediated synthesis strategy and promotes the application of machine learning toward the design and optimization of new zeolites.展开更多
基金National Key Research and Development Program of China (No. 2016YFB0701100)the National Natural Science Foundation of China (51802015)+1 种基金the Fundamental Research Funds for the Central Universities (FRF-TP-16-028A1)Program of Young Scholar sponsored by Beijing Organization Department (2017000020124G090) for financial support
文摘Electrochemical reduction of water to hydrogen holds great promise for clean energy,while its widespread application relies on the development of efficient catalysts with large surface area,abundant exposed active sites and superior electron conductivity.Herein,we report a facile strategy to configure an electrocatalyst composed of cobalt phosphide and rhodium uniformly anchored on reduced graphene oxide for hydrogen generation.The hybrids effectively integrate the exposed active sites,electron conductivity and synergistic effect of the catalyst.Electrochemical tests exhibit that the catalyst shows superior hydrogen evolution reaction catalytic activity and stability,with a small Tafel slope of 43 m V dec-1.Overpotentials as low as 29 and 72 mV are required to achieve current densities of 2 and 10 mA cm-2in 0.5M H2SO4,respectively.The hybrid constitution with highly active sites on conductive substrate is a new strategy to synthesize extremely efficient electrocatalysts.Especially,the efficient synergistic effect among cobalt phosphide,rhodium and reduced graphene oxide provides a novel approach for configuring electrocatalysts with high electron efficiency.
基金supported by the National Natural Science Foundation of China(51972024,51702013,51902025)the Fundamental Research Funds for the Central Universities(FRF-BD-20-07A,2019NTST29)+1 种基金the Scientific and Technological Innovation Foundation of Shunde Graduate School,University of Science and Technology Beijing(BK19AE029)funding from China Scholarship Council。
文摘Over the past decades, the energy and concomitant environment issues, such as energy shortage, air pollution and global warming, have been becoming increasingly striking world-wide challenges [1,2]. Such a dilemma in turn appeals to the development and employment of clean and renewable energy.
基金National Key Research and Development Program of China,Grant/Award Number:2021YFB3500700SINOPEC Research Institute of Petroleum Processing+3 种基金Natural Science Foundation of Guangdong Province of China,Grant/Award Number:2022A1515011918Scientific and Technological Innovation Foundation of Shunde Graduate SchoolUniversity of Science and Technology Beijing,Grant/Award Number:BK20AE003Fundamental Research Funds for the Central Universities,Grant/Award Number:FRF-IDRY-20-004。
文摘Simultaneous achievement of constructing mesopores and eliminating anatase is a long-term pursuit for enhancing the catalytic performance of TS-1.Here,we developed an aromatic compounds-mediated synthesis method to prepare anatase-free and hierarchical TS-1 for olefin epoxidation.A series of hierarchical TS-1 zeolites were prepared by introducing aromatic compounds containing different functional groups via the crystallization process.The formation of intercrystalline mesopores and insertion of titanium into framework were facilitated at different extent.The synergistic coordination of carboxyl and hydroxyl in aromatic compounds with Ti(OH)4 realizes the uniform distribution of titanium species and eliminates the generation of anatase.Noteworthily,eight machine learning models were trained to reveal the mechanism of additive functional groups and preparation conditions on anatase formation and microstructure optimization.The prediction accuracy of most models can reach more than 80%.Benefiting from the larger mesopore volumes(0.37 cm3⋅g−1)and higher content of framework Ti species,TS-DHBDC-48h samples exhibit a higher catalytic performance than other zeolites,giving 1-hexene conversion of 49.3%and 1,2-epoxyhenane selectivity of 99.9%.The paper provides a facile aromatic compounds-mediated synthesis strategy and promotes the application of machine learning toward the design and optimization of new zeolites.
