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CuPd alloy decorated SnNb2O6 nanosheets as a multifunctional photocatalyst for semihydrogenation of phenylacetylene under visible light
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2021-09-11 , DOI: 10.1016/j.cej.2021.132018
Zhiwen Wang 1 , Huan Wang 1 , Yingzhang Shi 1 , Cheng Liu 1 , Ling Wu 1, 2
Affiliation  

Bimetallic alloy of CuPd nanoclusters decorated SnNb2O6 nanosheets (CuPd/SN) as a multifunctional photocatalyst has been constructed successfully. Compared with SN, CuPd/SN achieves an excellent performance for semihydrogenation of phenylacetylene under visible light irradiation. Especially, CuPd/SN with the Cu:Pd molar ratio of 3:1 exhibits the highest catalytic conversion efficiency for phenylacetylene (99.6%) with high selectivity of phenylethylene (99.4%). In situ FTIR result reveals that SN could activate phenylacetylene via a C≡C→Nb π-bonded coordination which improves the selectivity of phenylethylene. Experiment results indicate that atom Pd in alloy is responsible for dissociation H2, while Cu represses the overhydrogenation. Electrochemical measurements indicates that CuPd alloy on SN surface could greatly minimize the recombination of photogenerated electron−hole pairs. The separated electrons further facilitate the production of active H. Hydrogen spillover would transfer active H to Nb site for phenylacetylene semihydrogenation. Finally, a synergetic catalytic mechanism is deeply discussed at molecule scale. This work would provide a deep insight for designing a multifunctional photocatalyst.



中文翻译:

CuPd合金装饰的SnNb2O6纳米片作为多功能光催化剂用于可见光下苯乙炔的半氢化

CuPd纳米团簇的双金属合金装饰SnNb 2 O 6纳米片(CuPd/SN)作为多功能光催化剂已成功构建。与SN相比,CuPd/SN在可见光照射下实现了苯乙炔半氢化的优异性能。特别是,Cu:Pd摩尔比为3:1的CuPd/SN对苯乙炔的催化转化效率最高(99.6%),对苯乙炔的选择性高(99.4%)。原位 FTIR 结果表明,SN 可以通过 C≡C→Nb π 键配位活化苯乙炔,从而提高苯乙炔的选择性。实验结果表明,合金中的原子 Pd 负责解离 H 2,而 Cu 抑制过度氢化。电化学测量表明,SN 表面上的 CuPd 合金可以大大减少光生电子 - 空穴对的复合。分离的电子进一步促进了活性 H 的产生。氢溢出会将活性 H 转移到 Nb 位点进行苯乙炔半氢化。最后,在分子尺度上深入讨论了协同催化机制。这项工作将为设计多功能光催化剂提供深刻的见解。

更新日期:2021-09-12
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