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作 者:邱爽 黄瑞 王红霞[1] 邓德会[2,3] QIU Shuang;HUANG Rui;WANG Hong-xia;DENG De-hui(College of Chemistry and Chemical Engineering,Harbin Normal University,Harbin 150025,China;State Key Laboratory of Catalysis,Collaborative Innovation Center of Chemistry for Energy Materials,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China;Zhang Dayu School of Chemistry,Dalian University of Technology,Dalian 116024,China)
机构地区:[1]哈尔滨师范大学化学化工学院,黑龙江哈尔滨150025 [2]中国科学院大连化学物理研究所能源材料化学协同创新中心,催化基础国家重点实验室,辽宁大连116023 [3]大连理工大学张大煜学院,辽宁大连116024
出 处:《分子科学学报》2021年第4期283-296,共14页Journal of Molecular Science
基 金:国家自然科学基金资助项目(21988101,21890753);中国科学院战略性先导科技专项资助项目(XDB36030200,XDA21010208);中国科学院前沿科学重点研究项目(QYZDB-SSWJSC020);中国科学技术部国家重点研究发展计划资助项目(2016YFA0204100,2016YFA0200200)。
摘 要:氨不仅是一种重要的化工原料,还是一种潜在的储氢能源载体.传统的Haber-Bosch合成氨工艺通常需要较高的温度和压力来解离强的N≡N键(945 kJ·mol^(-1)).因此,开发在温和条件下使用的高效合成氨催化剂引起了广泛关注.本文综述了负载型钌基催化剂、金属间化合物、金属氮化物和金属氢化物在温和条件下合成氨的研究进展,希望通过相应构效关系的关联,能给读者以启迪,更好地理解合成氨催化剂在氨合成过程中的作用,为新型合成氨催化剂的设计提供一定的理论指导.Ammonia is not only an important chemical raw material, but also a potential energy carrier for hydrogen storage. In conventional Haber-Bosch ammonia synthesis process, higher temperature and pressure operating conditions are usually required because of the dissociation of strong N≡N bond(945 kJ·mol^(-1)). Therefore, exploring efficient catalysts used under mild conditions has attracted intensive attention in the field of ammonia synthesis. In this paper, the research progress of supported ruthenium-based catalysts, intermetallic compounds, metal nitrides and metal hydrides for ammonia synthesis under mild conditions are summarized, aiming to provide some theoretical guidance for the design of efficient ammonia synthesis catalyst by constructing logical structure-property relationship between catalyst and ammonia synthesis. Carbon carriers, metal oxides and electrides have often been used as supports for loading Ru catalyst, and their structure and potential effect in ammonia synthesis will be given a brief introduction in this review. Compared with carbon materials like activated carbon, mesoporous carbon and carbon nanotubes, electrides and metal oxides especially those rare earth metal oxides and perovskite oxides as well as their derivatives, oxyhydroxides and oxynitride-hydrides, have demonstrated more positive effect on electron transfer from carrier to Ru catalyst, which make it easier to dissociate N≡N bond through back-donation of electrons from the d orbital of Ru to the antibonding π orbital of N2, consequently the ammonia synthesis activity is enhanced. Electrides are the materials with special structure that accommodate a certain amount of electrons within the interstitial space between cations, and these electrons are highly mobile in crystal because they are not bound to any atom in the framework. Moreover, the reversible hydrogen storage capacity possessed by electrides can also inhibit the hydrogen poisoning phenomenon of ruthenium, as a result, improved stability of Ru catalysts for ammoni
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