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Controllable in Situ Surface Restructuring of Cu Catalysts and Remarkable Enhancement of Their Catalytic Activity
He, Xiaohui1,2; Wang, Yong3,4; Zhang, Xun3,4; Dong, Mei5; Wang, Guofu5; Zhang, Bingsen6; Niu, Yiming6; Yao, Siyu1; He, Xin1; Liu, Haichao1
通讯作者Liu, Haichao(hcliu@pku.edu.cn)
2019-03-01
发表期刊ACS CATALYSIS
ISSN2155-5435
卷号9期号:3页码:2213-2221
摘要Supported metal catalysts play a pivotal role in the production of fuels and chemicals and environmental remediation. However, identification and tailoring of the active metal sites on these catalysts still remain a formidable challenge, primarily due to their dynamic nature in catalytic reactions. Here, we report a simple and effective strategy for tuning supported Cu nanoparticles via controllable in situ surface restructuring to form coordinatively more unsaturated Cu sites, which exhibit a 4-fold increase in catalytic turnover rate and high stability, as probed by the ethanol dehydrogenation reaction. In situ measurements by transmission electron microscopy and X-ray absorption spectroscopy reveal intense phase transformation and consequent dynamic restructuring of Cu nanoparticles, induced by oxidation with temporarily added nitrous oxide and subsequent reduction under reaction conditions. Such restructuring is precisely controlled at the Cu surfaces without altering Cu dispersion, oxidation state, etc., enabling us to unambiguously identify the active sites during catalysis. This strategy, an alternative to many sophisticated synthesis methods, has been shown to be effective for engineering different Cu catalysts and in turn markedly enhancing their catalytic activity for a wide range of reactions varying from alcohol dehydrogenation to methanol steam reforming.
关键词supported copper catalysts active metal site surface restructuring in situ characterization activity enhancement
资助者Natural Science Foundation of China ; National Key Research and Development Program of China
DOI10.1021/acscatal.8b04812
收录类别SCI
语种英语
资助项目Natural Science Foundation of China[21832001] ; Natural Science Foundation of China[21821004] ; Natural Science Foundation of China[21690081] ; Natural Science Foundation of China[21433001] ; Natural Science Foundation of China[51390474] ; Natural Science Foundation of China[91645103] ; Natural Science Foundation of China[21606260] ; National Key Research and Development Program of China[2016YFB0701100] ; National Key Research and Development Program of China[2016YFE0105700]
WOS研究方向Chemistry
WOS类目Chemistry, Physical
WOS记录号WOS:000460600600055
出版者AMER CHEMICAL SOC
引用统计
被引频次:48[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/132181
专题中国科学院金属研究所
通讯作者Liu, Haichao
作者单位1.Peking Univ, Beijing Natl Lab Mol Sci, Coll Chem & Mol Engn, Beijing 100871, Peoples R China
2.Sun Yat Sen Univ, Fine Chem Ind Res Inst, Sch Chem, Guangzhou 510275, Guangdong, Peoples R China
3.Zhejiang Univ, Sch Mat Sci & Engn, State Key Lab Silicon Mat, Hangzhou 310027, Zhejiang, Peoples R China
4.Zhejiang Univ, Sch Mat Sci & Engn, Ctr Electron Microscopy, Hangzhou 310027, Zhejiang, Peoples R China
5.Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Shanxi, Peoples R China
6.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China
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He, Xiaohui,Wang, Yong,Zhang, Xun,et al. Controllable in Situ Surface Restructuring of Cu Catalysts and Remarkable Enhancement of Their Catalytic Activity[J]. ACS CATALYSIS,2019,9(3):2213-2221.
APA He, Xiaohui.,Wang, Yong.,Zhang, Xun.,Dong, Mei.,Wang, Guofu.,...&Liu, Haichao.(2019).Controllable in Situ Surface Restructuring of Cu Catalysts and Remarkable Enhancement of Their Catalytic Activity.ACS CATALYSIS,9(3),2213-2221.
MLA He, Xiaohui,et al."Controllable in Situ Surface Restructuring of Cu Catalysts and Remarkable Enhancement of Their Catalytic Activity".ACS CATALYSIS 9.3(2019):2213-2221.
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