郑州大学臧双全团队报道了金属簇的电聚合为提高催化性能建立了一个多功能平台。相关研究成果于2022年1月3日发表在《德国应用化学》。

原子精确的金属团簇作为高效催化剂具有很大的吸引力，但在催化过程中会出现连续的效率失活。

该文中，研究人员开发了一种有效的策略，该策略通过将金属簇电聚合（EP）成杂化材料来提高催化性能。基于咔唑配体保护，制备了三种聚合金属簇杂化材料，即聚Cu14cba、聚Cu6Au6 cbz和聚Cu6Ag4 cbz。与孤立的金属团簇相比，EP后固定在双咔唑网络上的金属团簇显著提高了它们的电子转移能力和长期循环利用能力，从而提高了催化性能。

作为概念证明，聚Cu14 cba被评估为将硝酸盐（NO^3-）还原为氨（NH₃）的电催化剂，与具有良好耐久性的Cu 14 cba相比，其NH₃产率提高了约4倍，法拉第效率提高了约2倍。类似地，聚Cu6Au6cbz对化学战模拟物的光催化降解效率是簇合物的10倍。

附：英文原文

Title: Electropolymerization of Metal Clusters Establishing a Versatile Platform for Enhanced Catalysis Performance

Author: Yi-Man Wang, Jin-Meng Cai, Qian-You Wang, Yao Li, Zhen Han, Si Li, Chun-Hua Gong, Shan Wang, Shuang-Quan Zang, Thomas C. W. Mak

Issue&Volume: 2022-01-03

Abstract: Atomically-precise metal clusters are attractive as highly-efficient catalysts, but suffer from continuous efficiency deactivation in the catalytic process. Here, we report the development of an efficient strategy that enhance catalytic performance by electropolymerization (EP) of metal clusters into hybrid material. Based on carbazole ligand protection, three polymerized metal-cluster hybrid materials, namely  Poly-Cu  14  cba  ,  Poly-Cu  6  Au  6  cbz  and  Poly-Cu  6  Ag  4  cbz  , were prepared. Compared with isolated metal clusters, metal clusters immobilizing on biscarbazole network after EP significantly improved their electron-transfer ability and long-term recyclability, resulting in higher catalytic performance. As a proof-of-concept,  Poly-Cu  14  cba  was evaluated as an electrocatalyst for reducing nitrate (NO  3  -  ) to ammonia (NH  3  ), which exhibited ~4-fold NH  3  yield rate and ~2-fold Faraday efficiency enhancement compared to that of  Cu  14  cba  with good durability. Similarly,  Poly-Cu  6  Au  6  cbz  showed 10-times higher photocatalytic efficiency towards chemical warfare simulants degradation than the cluster counterpart.

DOI: 10.1002/anie.202114538

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202114538