Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-mi...Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-milling method for highly active and selective hydrogenation of CO_(2) to value-added hydrocarbons.When reacted at 320℃,1.0 MPa and 9600 mL h^(-1) g_(cat)^(-1),the selectivity to light olefin(C_(2)^(=)-C_(4)^(=)) and C_(5)+ species achieves 57.3% and 22.3%,respectively,at a CO_(2) co nversion of 31.4%,which is superior to previous Fe-based catalysts.The CO_(2) activation can be promoted by the CoFe phase formed by reactive ball milling of the Fe-Co_(3)O_(4) mixture,and the in-situ Co_(2)C and Fe_(5)C_(2) formed during hydrogenation are beneficial for the C-C coupling reaction.The initial C-C coupling is related to the combination of CO species with the surface carbon of Fe/Co carbides,and the sustained C-C coupling is maintained by self-recovery of defective carbides.This new strategy contributes to the development of efficient catalysts for the hydrogenation of CO_(2) to value-added hydrocarbons.展开更多
The copper-cobalt based catalysts were effective for higher alcohol synthesis, the surface state of the catalysts and the nature of the active sites were investigated by using XPS and XAES spectra, and some strong int...The copper-cobalt based catalysts were effective for higher alcohol synthesis, the surface state of the catalysts and the nature of the active sites were investigated by using XPS and XAES spectra, and some strong interactions were also observed, in each of the three cases, (after calcination, after reduction, and during the syngas reaction).展开更多
化石燃料的燃烧导致大气中二氧化碳(CO_(2))的浓度迅速上升,并引发了严重的能源、环境危机。由可再生电力驱动的电催化CO_(2)还原为增值化学品和燃料是解决当前化石燃料枯竭的一种有效方法。采用“一锅法”制备了磷(P)修饰的高分散性“...化石燃料的燃烧导致大气中二氧化碳(CO_(2))的浓度迅速上升,并引发了严重的能源、环境危机。由可再生电力驱动的电催化CO_(2)还原为增值化学品和燃料是解决当前化石燃料枯竭的一种有效方法。采用“一锅法”制备了磷(P)修饰的高分散性“钴-氮-碳”(Co-N-C/P)催化剂,通过扫描电子显微镜(SEM)、X射线衍射(XRD)、拉曼光谱(Raman)和X射线光电子能谱(XPS)等手段对催化剂的形貌、元素分布、缺陷程度、表面元素价态及配位结构进行了表征,并考察了其在H型电解槽中电催化CO_(2)还原为CO的性能。测试结果表明,所制备的Co-N-C/P催化剂在-0.9 V vs.RHE的外加电位下具有97.0%的CO法拉第效率(FE_(CO)),电流密度为4.58 mA/cm^(2),并可以进行26 h的稳定性测试。与Co-N-C催化剂相比,P的掺杂更有利于Co原子在碳黑基底上的良好分散,相应的FE_(CO)提高了约38.9%,说明P的掺杂有效提高了Co-N-C催化剂的电催化CO_(2)还原为CO的性能。展开更多
基金supported by the Foundation of Shaanxi Educational Committee (2010JK608)the Research Foundation of XATU (204-000092)supported by the National Natural Science Foundation of China (205903603)
基金supported by the National Natural Science Foundation of China (22008098, 21978156, 42002040)the Program for Innovative Research Team (in Science and Technology) in University of Henan Province (21IRTSTHN004)+1 种基金the Program for Science & Technology Innovation Talents in Universities of Henan Province (22HASTIT008)the Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering (2022-K34)。
文摘Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-milling method for highly active and selective hydrogenation of CO_(2) to value-added hydrocarbons.When reacted at 320℃,1.0 MPa and 9600 mL h^(-1) g_(cat)^(-1),the selectivity to light olefin(C_(2)^(=)-C_(4)^(=)) and C_(5)+ species achieves 57.3% and 22.3%,respectively,at a CO_(2) co nversion of 31.4%,which is superior to previous Fe-based catalysts.The CO_(2) activation can be promoted by the CoFe phase formed by reactive ball milling of the Fe-Co_(3)O_(4) mixture,and the in-situ Co_(2)C and Fe_(5)C_(2) formed during hydrogenation are beneficial for the C-C coupling reaction.The initial C-C coupling is related to the combination of CO species with the surface carbon of Fe/Co carbides,and the sustained C-C coupling is maintained by self-recovery of defective carbides.This new strategy contributes to the development of efficient catalysts for the hydrogenation of CO_(2) to value-added hydrocarbons.
文摘The copper-cobalt based catalysts were effective for higher alcohol synthesis, the surface state of the catalysts and the nature of the active sites were investigated by using XPS and XAES spectra, and some strong interactions were also observed, in each of the three cases, (after calcination, after reduction, and during the syngas reaction).
文摘化石燃料的燃烧导致大气中二氧化碳(CO_(2))的浓度迅速上升,并引发了严重的能源、环境危机。由可再生电力驱动的电催化CO_(2)还原为增值化学品和燃料是解决当前化石燃料枯竭的一种有效方法。采用“一锅法”制备了磷(P)修饰的高分散性“钴-氮-碳”(Co-N-C/P)催化剂,通过扫描电子显微镜(SEM)、X射线衍射(XRD)、拉曼光谱(Raman)和X射线光电子能谱(XPS)等手段对催化剂的形貌、元素分布、缺陷程度、表面元素价态及配位结构进行了表征,并考察了其在H型电解槽中电催化CO_(2)还原为CO的性能。测试结果表明,所制备的Co-N-C/P催化剂在-0.9 V vs.RHE的外加电位下具有97.0%的CO法拉第效率(FE_(CO)),电流密度为4.58 mA/cm^(2),并可以进行26 h的稳定性测试。与Co-N-C催化剂相比,P的掺杂更有利于Co原子在碳黑基底上的良好分散,相应的FE_(CO)提高了约38.9%,说明P的掺杂有效提高了Co-N-C催化剂的电催化CO_(2)还原为CO的性能。