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Colloidal Co single-atom catalyst: a facile synthesis strategy and high catalytic activity for hydrogen generation
Green Chemistry ( IF 9.8 ) Pub Date : 2020/01/24 , DOI: 10.1039/c9gc03477c
Junkai Wang 1, 2, 3, 4, 5 , Zhenxia Huang 1, 2, 3, 4, 5 , Lilin Lu 1, 2, 3, 4 , Quanli Jia 6, 7, 8, 9 , Liang Huang 1, 2, 3, 4 , Shuai Chang 1, 2, 3, 4 , Mingyang Zhang 1, 2, 3, 4 , Zuotai Zhang 4, 10, 11, 12 , Sun Li 4, 10, 11, 12 , Dongsheng He 4, 11, 12, 13 , Wenhao Wu 1, 2, 3, 4 , Shaowei Zhang 14, 15, 16, 17, 18 , Naoki Toshima 19, 20, 21, 22 , Haijun Zhang 1, 2, 3, 4
Affiliation  

Developing highly active single-atom catalysts is one of the most significant issues for future renewable energy technologies. Here we present a facile but effective and efficient strategy for synthesizing colloidal Co single-atom catalysts with excellent catalytic activity using a copolymer, poly(isobutylene-alt-maleic anhydride) (ISOBAM-104), as a stabilizing agent. The catalytic activity of the as-prepared colloidal single-atom catalyst for hydrogen generation from hydrolysis of KBH4 in an alkaline solution was as high at about 14 300 mL-H2 min−1 g-Co−1, which was even higher than that of its Pt, Pd or Rh counterpart. Such a high catalytic activity of the colloidal catalyst was attributable to the in situ formed and well-stabilized Co single-atoms whose existence was confirmed by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy. Moreover, quantum chemical calculations reveal that ISOBAM-104 has a higher binding energy with the Co catalyst than with the well-known conventional protective agents, including poly(N-vinyl-2-pyrrolidone), starch, carboxymethylcellulose sodium, polyvinyl alcohol, sodium polyacrylate and polyethylene glycol. In addition, the use of as-prepared Co catalysts resulted in a much lowered barrier for the dissociation reaction of BH4 than in the cases of using Pt, Pd and Rh counterpart catalysts.

中文翻译:

胶态Co单原子催化剂:一种简便的合成策略和高催化活性的产氢

开发高活性单原子催化剂是未来可再生能源技术最重要的问题之一。这里,我们提出一种使用共聚物,聚(异丁烯合成的胶体CO单原子催化剂具有优良的催化活性的简便而有效的和高效的策略ALT -马来酸酐)(ISOBAM-104),作为稳定剂。所制备的胶体单原子催化剂对碱性溶液中KBH 4水解产生氢的催化活性高达约14300 mL-H 2 min -1 g-Co -1,甚至高于其对应的Pt,Pd或Rh的金属。胶体催化剂的这种高催化活性归因于原位形成且稳定的Co单原子,其存在通过像差校正的高角度环形暗场扫描透射电子显微镜得以证实。此外,量子化学计算表明,ISOBAM-104与Co催化剂的结合能比众所周知的常规保护剂(包括聚N-乙烯基-2-吡咯烷酮),淀粉,羧甲基纤维素钠,聚乙烯醇,聚丙烯酸酯和聚乙二醇。另外,使用所制备的Co催化剂的导致了BH的离解反应更降低的挡板4 -比使用铂,钯和Rh对方催化剂的情况下。
更新日期:2020-02-24
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