Diatomic Palladium Catalyst for Enhanced Photocatalytic Water-Donating Transfer Hydrogenation

doi:10.1021/jacs.4c15235

	Diatomic Palladium Catalyst for Enhanced Photocatalytic Water-Donating Transfer Hydrogenation
	Zhao, En 1; Morales-Vidal, Jordi 2; Yang, Yue3 ; Mitchell, Sharon 4; Zhu, Yinlong 5; Hu, Zhiwei 6; Chen, Jin-Ming 7; Haw, Shu-Chih 8; Chan, Ting-Shan 8; Fan, Ziyi 1; Wang, Zhu-Jun3 ; Lopez, Nuria 2; Perez-Ramirez, Javier 4; Chen, Zupeng 1
	2025-01-06
发表期刊	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (IF:14.4[JCR-2023],14.8[5-Year])
ISSN	0002-7863
EISSN	1520-5126
卷号	147 期号:2 页码:2029-2036
DOI	10.1021/jacs.4c15235
摘要	Diatomic catalysts (DACs) present unique opportunities for harnessing ensemble effects between adjacent metal atoms, thus, expanding the properties of single-atom catalysts (SACs). However, the precise preparation and characterization of this type of catalyst remains challenging. Following a precursor-preselected strategy, here, we report the synthesis of a carbon nitride-supported Pd-DAC, which achieves an excellent yield of 92% for photocatalytic water-donating transfer hydrogenation of 4-vinylphenol to 4-ethylphenol, far exceeding that of other metal species, including Pd single atoms (47%) and nanoparticles (1%). Combining transmission electron microscopy with standardized machine learning atom-detection methods confirms the stabilization of a substantial fraction of dimeric Pd species over carbon nitride. Density functional theory (DFT) simulations associate the outstanding performance of Pd-DAC to enhanced substrate activation in the hydrogenation path compared to Pd-SAC. The work provides criteria for DACs characterization and demonstrates a transfer hydrogenation application that is sustainable and eco-friendly over conventional hydrogenation technologies.
关键词	High resolution transmission electron microscopy Hydrogenation Palladium compounds Photocatalytic activity A-carbon Diatomics Ensemble effect Metal atoms Palladium catalyst Photo-catalytic Property Single-atoms Transfer hydrogenations ]+ catalyst
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收录类别	SCI ; EI
语种	英语
资助项目	Ministerio de Ciencia, Innovaci?n y Universidades[2023YFD2200505] ; National Key Research and Development Program of China[22202105] ; National Natural Science Foundation of China[21KJA150003] ; Natural Science Foundation of Jiangsu Higher Education Institutions of China[JSSCTD202345] ; Innovation and Entrepreneurship Team Program of Jiangsu Province[PID2021-122516OB-I00] ; Generalitat de Catalunya[2023 CLIMA 00105]
WOS研究方向	Chemistry
WOS类目	Chemistry, Multidisciplinary
WOS记录号	WOS:001390554200001
出版者	AMER CHEMICAL SOC
EI入藏号	20250317715022
EI主题词	Carbon nitride
EI分类号	1301.3.1 Microscopy ; 202.7.1.4 Palladium and Alloys ; 802.2 Chemical Reactions ; 804.1 Organic Compounds
原始文献类型	Journal article (JA)
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/470977
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_王竹君组
通讯作者	Wang, Zhu-Jun; Lopez, Nuria; Perez-Ramirez, Javier; Chen, Zupeng
作者单位	1.Nanjing Forestry Univ, Coll Chem Engn, Jiangsu Coinnovat Ctr Efficient Proc & Utilizat Fo, Int Innovat Ctr Forest Chem & Mat,Jiangsu Prov Key, Nanjing 210037, Peoples R China 2.Barcelona Inst Sci & Technol, Inst Chem Res Catalonia ICIQ CERCA, Tarragona 43007, Spain 3.Shanghai Tech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China 4.Swiss Fed Inst Technol, Inst Chem & Bioengn, Dept Chem & Appl Biosci, CH-8093 Zurich, Switzerland 5.Nanjing Univ Aeronaut & Astronaut, Inst Frontier Sci, Nanjing 210016, Peoples R China 6.Max Planck Inst Chem Phys Solids, D-01187 Dresden, Germany 7.Natl Yang Ming Chiao Tung Univ, Dept Electrophys, Hsinchu 300, Taiwan 8.Natl Synchrotron Radiat Res Ctr, Hsinchu 30076, Taiwan
通讯作者单位	物质科学与技术学院
推荐引用方式 GB/T 7714	Zhao, En,Morales-Vidal, Jordi,Yang, Yue,et al. Diatomic Palladium Catalyst for Enhanced Photocatalytic Water-Donating Transfer Hydrogenation[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2025,147(2):2029-2036.
APA	Zhao, En.,Morales-Vidal, Jordi.,Yang, Yue.,Mitchell, Sharon.,Zhu, Yinlong.,...&Chen, Zupeng.(2025).Diatomic Palladium Catalyst for Enhanced Photocatalytic Water-Donating Transfer Hydrogenation.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,147(2),2029-2036.
MLA	Zhao, En,et al."Diatomic Palladium Catalyst for Enhanced Photocatalytic Water-Donating Transfer Hydrogenation".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 147.2(2025):2029-2036.