Homolytic H<sub>2</sub> dissociation for enhanced hydrogenation catalysis on oxides

doi:10.1038/s41467-024-44711-7

	Homolytic H₂ dissociation for enhanced hydrogenation catalysis on oxides
	Yang, Chengsheng 1; Ma, Sicong 2; Liu, Yongmei 1; Wang, Lihua 3; Yuan, Desheng 1; Shao, Wei-Peng4 ; Zhang, Lunjia4 ; Yang, Fan4 ; Lin, Tiejun 5; Ding, Hongxin 1; He, Heyong 1; Liu, Zhi-Pan 1,2; Cao, Yong 1; Zhu, Yifeng 1; Bao, Xinhe 1,6
	2024-01-15
发表期刊	NATURE COMMUNICATIONS (IF:14.7[JCR-2023],16.1[5-Year])
EISSN	2041-1723
卷号	15 期号:1
发表状态	已发表
DOI	10.1038/s41467-024-44711-7
摘要	The limited surface coverage and activity of active hydrides on oxide surfaces pose challenges for efficient hydrogenation reactions. Herein, we quantitatively distinguish the long-puzzling homolytic dissociation of hydrogen from the heterolytic pathway on Ga2O3, that is useful for enhancing hydrogenation ability of oxides. By combining transient kinetic analysis with infrared and mass spectroscopies, we identify the catalytic role of coordinatively unsaturated Ga3+ in homolytic H-2 dissociation, which is formed in-situ during the initial heterolytic dissociation. This site facilitates easy hydrogen dissociation at low temperatures, resulting in a high hydride coverage on Ga2O3 (H/surface Ga3+ ratio of 1.6 and H/OH ratio of 5.6). The effectiveness of homolytic dissociation is governed by the Ga-Ga distance, which is strongly influenced by the initial coordination of Ga3+. Consequently, by tuning the coordination of active Ga3+ species as well as the coverage and activity of hydrides, we achieve enhanced hydrogenation of CO2 to CO, methanol or light olefins by 4-6 times.
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收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China (National Science Foundation of China)[2022YFA1503804] ; Ministry of Science and Technology of China["22102033","22272031"] ; National Natural Science Foundation of China["22ZR1408000","22QA1401300"] ; Science & Technology Commission of Shanghai Municipality[BX20220090] ; China National Postdoctoral Program for Innovative Talents[2022M710740] ; China Postdoctoral Science Foundation[20720220008] ; Fundamental Research Funds for the Central Universities[KLLCCSE-202201]
WOS研究方向	Science & Technology - Other Topics
WOS类目	Multidisciplinary Sciences
WOS记录号	WOS:001143918100021
出版者	NATURE PORTFOLIO
引用统计	正在获取...
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/349934
专题	物质科学与技术学院物质科学与技术学院_博士生物质科学与技术学院_PI研究组_杨帆组
通讯作者	Ma, Sicong; Zhu, Yifeng; Bao, Xinhe
作者单位	1.Fudan Univ, Collaborat Innovat Ctr Chem Energy Mat, Dept Chem, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai 200438, Peoples R China 2.Chinese Acad Sci, Shanghai Inst Organ Chem, Key Lab Synthet & Selfassembly Chem Organ Funct Mo, Shanghai 200032, Peoples R China 3.Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China 4.Shanghai Tech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China 5.Chinese Acad Sci, Shanghai Adv Res Inst, Key Lab Low Carbon Convers Sci & Engn, Shanghai 201210, Peoples R China 6.Chinese Acad Sci, Dalian Inst Chem Phys, Collaborat Innovat Ctr Chem Energy Mat, State Key Lab Catalysis,Natl Lab Clean Energy, Dalian 116023, Peoples R China
推荐引用方式 GB/T 7714	Yang, Chengsheng,Ma, Sicong,Liu, Yongmei,et al. Homolytic H₂ dissociation for enhanced hydrogenation catalysis on oxides[J]. NATURE COMMUNICATIONS,2024,15(1).
APA	Yang, Chengsheng.,Ma, Sicong.,Liu, Yongmei.,Wang, Lihua.,Yuan, Desheng.,...&Bao, Xinhe.(2024).Homolytic H₂ dissociation for enhanced hydrogenation catalysis on oxides.NATURE COMMUNICATIONS,15(1).
MLA	Yang, Chengsheng,et al."Homolytic H₂ dissociation for enhanced hydrogenation catalysis on oxides".NATURE COMMUNICATIONS 15.1(2024).