Fully exposed Pt clusters for efficient catalysis of multi-step hydrogenation reactions | |
Si, Yang1,2; Jiao, Yueyue3,4,5; Wang, Maolin6; Xiang, Shengling7,8; Diao, Jiangyong2; Chen, Xiaowen1,2; Chen, Jiawei1,2; Wang, Yue2,9; Xiao, Dequan10; Wen, Xiaodong3,4; Wang, Ning7,8,9; Ma, Ding6; Liu, Hongyang1,2 | |
通讯作者 | Diao, Jiangyong(jydiao@imr.ac.cn) ; Ma, Ding(dma@pku.edu.cn) ; Liu, Hongyang(liuhy@imr.ac.cn) |
2024-06-07 | |
发表期刊 | NATURE COMMUNICATIONS
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卷号 | 15期号:1页码:10 |
摘要 | For di-nitroaromatics hydrogenation, it is a challenge to achieve the multi-step hydrogenation with high activity and selectivity due to the complexity of the process involving two nitro groups. Consequently, many precious metal catalysts suffer from low activity for this multi-step hydrogenation reaction. Herein, we employ a fully exposed Pt clusters catalyst consisting of an average of four Pt atoms on nanodiamond@graphene (Ptn/ND@G), demonstrating excellent catalytic performance for the multi-step hydrogenation of 2,4-dinitrotoluene. The TOF (40647 h-1) of Ptn/ND@G is significantly superior to that of single Pt atoms catalyst, Pt nanoparticles catalyst, and even all the known catalysts. Density functional theory calculations and absorption experiments reveal that the synergetic interaction between the multiple active sites of Ptn/ND@G facilitate the co-adsorption/activation of reactants and H2, as well as the desorption of intermediates/products, which is the key for the higher catalytic activity than single Pt atoms catalyst and Pt nanoparticles catalyst. Hydrogenating di-nitroaromatics with high activity and selectivity is challenging due to the process's complexity. Here the authors present a fully exposed Pt clusters catalyst for 2,4-dinitrotoluene hydrogenation, suggesting that the synergy between multiple active sites and moderate adsorption behavior is crucial for the high catalytic activity. |
资助者 | National Key RD Program of China (2022YFA1504500, 2022YFB4003100, 2021YFA1502802), the National Natural Science Foundation of China (92145301, U21B2092, 21961160722, 91845201, 22072162), the International Partnership Program of Chinese Academy of Sciences ; National Key R&D Program of China ; National Natural Science Foundation of China ; International Partnership Program of Chinese Academy of Sciences ; Shenyang Young Talents Program ; Dalian National Lab for Clean Energy (DNL Cooperation Fund) ; China Petroleum & Chemical Corporation ; Shanghai Synchrotron Radiation Facility (SSRF) ; Tencent Foundation through the XPLORER PRIZE |
DOI | 10.1038/s41467-024-49083-6 |
收录类别 | SCI |
语种 | 英语 |
资助项目 | National Key RD Program of China (2022YFA1504500, 2022YFB4003100, 2021YFA1502802), the National Natural Science Foundation of China (92145301, U21B2092, 21961160722, 91845201, 22072162), the International Partnership Program of Chinese Academy of Sciences[2022YFA1504500] ; National Key RD Program of China (2022YFA1504500, 2022YFB4003100, 2021YFA1502802), the National Natural Science Foundation of China (92145301, U21B2092, 21961160722, 91845201, 22072162), the International Partnership Program of Chinese Academy of Sciences[2022YFB4003100] ; National Key RD Program of China (2022YFA1504500, 2022YFB4003100, 2021YFA1502802), the National Natural Science Foundation of China (92145301, U21B2092, 21961160722, 91845201, 22072162), the International Partnership Program of Chinese Academy of Sciences[2021YFA1502802] ; National Key R&D Program of China[22072162] ; National Key R&D Program of China[2202213] ; National Key R&D Program of China[92145301] ; National Key R&D Program of China[U21B2092] ; National Key R&D Program of China[21961160722] ; National Key R&D Program of China[91845201] ; National Natural Science Foundation of China[172GJHZ2022028MI] ; International Partnership Program of Chinese Academy of Sciences[RC210435] ; Shenyang Young Talents Program[202001] ; Dalian National Lab for Clean Energy (DNL Cooperation Fund)[420043-2] ; China Petroleum & Chemical Corporation ; Shanghai Synchrotron Radiation Facility (SSRF) ; Tencent Foundation through the XPLORER PRIZE |
WOS研究方向 | Science & Technology - Other Topics |
WOS类目 | Multidisciplinary Sciences |
WOS记录号 | WOS:001244296600009 |
出版者 | NATURE PORTFOLIO |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://ir.imr.ac.cn/handle/321006/187444 |
专题 | 中国科学院金属研究所 |
通讯作者 | Diao, Jiangyong; Ma, Ding; Liu, Hongyang |
作者单位 | 1.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 3.Chinese Acad Sci, State Key Lab Coal Convers, Inst Coal Chem, Taiyuan 030001, Peoples R China 4.Synfuels China Co Ltd, Natl Energy Ctr Coal Clean Fuel, Beijing 100871, Peoples R China 5.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 6.Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, New Cornerstone Sci Lab, Beijing 100871, Peoples R China 7.Hong Kong Univ Sci & Technol, Dept Phys, Kowloon, Hong Kong, Peoples R China 8.Hong Kong Univ Sci & Technol, Ctr Quantum Mat, Kowloon, Hong Kong, Peoples R China 9.Liaoning Univ, Dept Chem, 66 Chongshan Rd, Shenyang 110036, Liaoning, Peoples R China 10.Univ New Haven, Ctr Integrat Mat Discovery, Dept Chem & Chem Engn, West Haven, CT 06516 USA |
推荐引用方式 GB/T 7714 | Si, Yang,Jiao, Yueyue,Wang, Maolin,et al. Fully exposed Pt clusters for efficient catalysis of multi-step hydrogenation reactions[J]. NATURE COMMUNICATIONS,2024,15(1):10. |
APA | Si, Yang.,Jiao, Yueyue.,Wang, Maolin.,Xiang, Shengling.,Diao, Jiangyong.,...&Liu, Hongyang.(2024).Fully exposed Pt clusters for efficient catalysis of multi-step hydrogenation reactions.NATURE COMMUNICATIONS,15(1),10. |
MLA | Si, Yang,et al."Fully exposed Pt clusters for efficient catalysis of multi-step hydrogenation reactions".NATURE COMMUNICATIONS 15.1(2024):10. |
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