材料科学
光催化
选择性
电子转移
Atom(片上系统)
甲醛
异核分子
吸附
催化作用
光化学
物理化学
核磁共振波谱
立体化学
有机化学
化学
嵌入式系统
计算机科学
作者
Bupmo Kim,Dayoung Kwon,Jin‐Ook Baeg,Muthu Austeria P,Geun Ho Gu,Jeong‐Hyeon Lee,Jeehun Jeong,Wooyul Kim,Wonyong Choi
标识
DOI:10.1002/adfm.202212453
摘要
Abstract The solar‐driven catalytic reduction of CO 2 to value‐added chemicals is under intensive investigation. The reaction pathway via *OCHO intermediate (involving CO 2 adsorbed through O‐binding) usually leads to the two‐electron transfer product of HCOOH. Herein, a single‐atom catalyst with dual‐atom‐sites featuring neighboring Sn(II) and Cu(I) centers embedded in C 3 N 4 framework is developed and characterized, which markedly promotes the production of HCHO via four‐electron transfer through the *OCHO pathway. The optimized catalyst achieves a high HCHO productivity of 259.1 µmol g −1 and a selectivity of 61% after 24 h irradiation, which is ascribed to the synergic role of the neighboring Sn(II)–Cu(I) dual‐atom sites that stabilize the target intermediates for HCHO production. Moreover, adsorbed *HCHO intermediate is detected by in situ Fourier transform infrared spectroscopy (CO stretches at 1637 cm −1 ). This study provides a unique example that controls the selectivity of the multi‐electron transfer mechanisms of CO 2 photoconversion using heteronuclear dual‐atom‐site catalyst to generate an uncommon product (HCHO) of CO 2 reduction.
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