N -Heterocyclic Carbene Gold Complexes in a Photocatalytic CO 2 Reduction Reaction
N -Heterocyclic Carbene Gold Complexes in a Photocatalytic CO 2 Reduction Reaction
复制标题
N-杂环卡宾金配合物在光催化CO 2 还原反应中的应用
DOI：
10.1021/acs.inorgchem.2c03487
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发表时间：
2022
影响因子：
4.6
通讯作者：
Delcamp, Jared H.
中科院分区：
文献类型：
--
作者：
Nugegoda, Dinesh;Tzouras, Nikolaos V.;Nolan, Steven P.;Delcamp, Jared H.
在光催化二氧化碳还原反应(PCO2RR)中，耐用和高选择性的分子催化剂的需求量很大。尽管多相金-二氧化碳还原催化剂对应的催化剂经常被研究，但分子金配合物在CO2RR流形中仍未被充分开发。在这篇报道中，一系列n-杂环卡宾(NHC)连接的金的配合物在PCO_2RR中被加入光敏剂(三(2-苯基吡啶)Ir，Ir(Ppy)_3)被评价。每个配合物都在有和没有添加活化剂的情况下进行研究，该活化剂用于在Au配合物上打开配位。结果表明，一种特别耐用的PCO2RR催化剂可持续>；100h，对CO有高的产物选择性。多相实验没有发现活性催化剂不均一的证据，并讨论了分子络合物的结构-活性关系。
Molecular catalysts that are durable and highly selective in the photocatalytic CO2reduction reaction (PCO2RR) are in high demand. Molecular gold complexes are underexplored in the CO2RR manifold despite heterogeneous gold–CO2reduction catalyst counterparts being frequently studied. In this report, a series ofN-heterocyclic carbene (NHC)-ligated Au complexes are evaluated in the PCO2RR with an added photosensitizer (tris(2-phenylpyridine)iridium, Ir(ppy)3). The complexes were each studied with and without an added activator used to open a coordination site on the Au complexes. Results show an example of an exceptionally durable PCO2RR catalyst lasting >100 h with high product selectivity for CO. Heterogeneity tests reveal no evidence of a nonhomogeneous active catalyst, and structure–activity relationships of the molecular complexes are discussed.