多相催化加氢反应中H2异裂解离的研究进展OACSTPCD
Research progress of H2 heterolysis in heterogeneous catalytic hydrogenation
多相催化加氢反应是制备高附加值燃料及化学品的重要途径,而H2异裂解离过程及其形成的氢化物(M—Hδ-)的化学性质与加氢反应活性和选择性密切相关.然而,由于多相催化剂表面结构复杂导致了H2异裂解离过程及M—Hδ-化学性质的多样性,为认识H2异裂解离及M—Hδ-的化学性质对加氢反应机理的调控规律带来了巨大挑战.综述了H2异裂解离的机理及M—Hδ-的化学性质,并介绍了常用于检测M—Hδ-的表征技术并分析了各自的优缺点.重点讨论了不同多相催化体系,如负载型金属催化剂、金属氧化物催化剂以及阴离子杂化金属催化剂中,H2异裂解离与催化剂活性位点结构之间的内在关系及其对加氢反应性能的优化,并提出了调控H2异裂解离的有效策略.最后,针对当前H2异裂解离及M—Hδ-研究面临的主要挑战进行了总结,同时对未来发展方向进行了展望.
Heterogeneous catalytic hydrogenation is an important approach for preparation of high-value-added fuels and chemicals,while the processes of H2 heterolysis and chemical properties of generated hydrides(M—Hδ-)are closely related to hydrogenation activity and selectivity.However,the complex surface structure of heterogeneous catalysts,which leads to a diversity of H2 heterolysis process and M—Hδ-chemical properties,poses a great challenge in understanding the regulation of H2 heterolysis and M—Hδ-chemical properties on the mechanism of hydrogenation reactions.The mechanism of H2 heterolysis and the chemical properties of M—Hδ-were reviewed,and the characterization techniques commonly used to detect M—Hδ-were presented and their advantages and disadvantages were analyzed.The internal relationship between H2 heterolysis and the structure of active site of catalysts in different heterogeneous catalytic systems,such as metal-supported catalysts,metal oxide catalysts and anionic hybrid metal catalysts,as well as the optimization of the performance of hydrogenation reaction were discussed,and effective strategies to regulate H2 heterolysis were proposed.Finally,the main challenges in the study of H2 heterolysis and M—Hδ-were summarized and future development directions were outlined.
姚正阳;王晓月;郭晓宏;赵勇杰;师文荣;李聪明
太原理工大学 省部共建煤基能源清洁高效利用国家重点实验室,山西 太原 030024
化学工程
加氢反应H2异裂解离氢化物催化剂多相催化
hydrogenation reactionH2 heterolysishydridecatalystheterogeneous catalysis
《低碳化学与化工》 2024 (001)
1-11 / 11
国家自然科学基金(21676176);山西省自然科学基金(20210302123143);山西省重点研发计划(202202090301013);大学生创新创业训练计划(20220095).
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