当前位置:科学网首页 > 小柯机器人 >详情
设计“分子连接”以传输光生电子,将二氧化碳还原为乙烷
作者:小柯机器人 发布时间:2026/3/19 13:52:06


近日,安徽师范大学王刚团队报道了设计“分子连接”以传输光生电子,将二氧化碳还原为乙烷。相关论文于2026年3月18日发表在《德国应用化学》杂志上。

电子的靶向传输是高效实现光还原过程的关键,这仍是当前研究面临的重大挑战。在光催化剂与金属活性位点之间构建“分子结”有望实现精确的定向电子转移。

研究组引入兼具巯基(─SH)和共轭吡啶环的2-巯基烟酸(H2L)作为中间体,构建连接Ni掺杂BiOCl(Ni/BOC)与金纳米粒子(Au NPs)的"分子结"(记为Ni/BOC-H2L-Au)。XPS和XAFS结果证实了Bi─S和Au─S键的存在,验证了Ni/BOC中Bi─H2L─Au"分子结"的成功构建。

由于Ni/BOC-H2L-Au的独特结构,其在CO2光还原中展现出优异性能。在无牺牲剂条件下,乙烷(C2H6)产率(155.4 µmol g−1 h−1)和选择性(85.8%)超过大多数已报道的光催化剂。理论与实验联合分析表明,"分子结"建立了定向电子转移路径(Ni/BOC→H2L→Au NPs),显著增强电荷分离效率并促进电子靶向富集于Au NPs活性位点,从而提升CO2光还原生成C2H6的效率。该工作为设计高效合成高附加值C2+产物的光催化剂提供了可行策略。

附:英文原文

Title: Engineered “Molecule-Junction” to Transport Photo-Generated Electrons for CO2 Reduction to Ethane

Author: Yan Wu, Xing Gao, Rui Yu, Chengyang Zhu, Dongyang Yu, Zaizhu Lou, Zhujie Li, Gang Wang

Issue&Volume: 2026-03-18

Abstract: Targeted transport of electrons is essential to enable the photoreduction process efficiently, which remains a significant challenge in current research. Constructing “molecule-junction” between photocatalyst and metal active sites is expected to achieve the precise directional electron transfer. 2-Mercaptonicotinic acid (H2L), with both sulfhydryl groups (─SH) and a conjugated pyridine ring, was introduced as the intermediary to build “molecule-junction” connecting Ni-doped BiOCl (Ni/BOC) and Au NPs (denoted as Ni/BOC-H2L-Au). XPS and XAFS results confirm the existence of Bi─S and Au─S bonds, which verify that the “molecule-junction” of Bi─H2L─Au have been successfully constructed in Ni/BOC. Due to the unique structure of Ni/BOC-H2L-Au, it showed excellent performance in CO2 photoreduction. In the absence of sacrificial agents, the ethane (C2H6) yield (155.4 μmol g1 h1) and selectivity (85.8%) exceeded most of the reported photocatalysts. The combined theoretical and experimental analysis demonstrates that the “molecule-junction” establishes a directional electron transfer pathway (Ni/BOC→H2L→Au NPs), which significantly enhances charge separation efficiency and promotes targeted electron accumulation at Au NPs active sites, thereby boosting C2H6 production via CO2 photoreduction. This work proposes a viable strategy for designing efficient photocatalysts for high-value C2+ product synthesis.

DOI: 10.1002/anie.2699441

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.2699441

期刊信息

Angewandte Chemie:《德国应用化学》,创刊于1887年。隶属于德国化学会,最新IF:16.823
官方网址:https://onlinelibrary.wiley.com/journal/15213773
投稿链接:https://www.editorialmanager.com/anie/default.aspx