Li Jun, Pan Wenfeng, Liu Qiaoyun, Chen Zhiquan, Chen Zhijie, Feng Xuezhen, Chen Hong
Henan Institute of Advanced Technology, Zhengzhou University, Zhengzhou 450052, China.
College of Chemistry, Zhengzhou University, Zhengzhou 450001, China.
J Am Chem Soc. 2021 May 5;143(17):6551-6559. doi: 10.1021/jacs.1c01109. Epub 2021 Apr 14.
Developing highly efficient photocatalysts to utilize solar radiation for converting CO into solar fuels is of great importance for energy sustainability and carbon neutralization. Herein, through an alkali-etching-introduced interface reconstruction strategy, a nanowire photocatalyst denoted as V-BiBrS, with rich Br and S dual-vacancies and surface Bi-O bonding introduced significant near-infrared (NIR) light response, has been developed. The as-obtained V-BiBrS nanowires exhibit a highly efficient metallic photocatalytic reduction property for converting CO into CHOH when excited solely under NIR light irradiation. Free of any cocatalyst and sacrificial agent, metallic defective V-BiBrS shows 2.3-fold higher CHOH generation than BiBrS nanowires. The detailed interfacial structure evolution and reaction mechanism have been carefully illustrated down to the atomic scale. This work provides a unique interfacial engineering strategy for developing high-performance sulfur-based NIR photocatalysts for photon reducing CO into alcohol for achieving high-value solar fuel chemicals, which paves the way for efficiently using the solar radiation energy extending to the NIR range to achieve the carbon neutralization goal.
开发高效光催化剂以利用太阳辐射将CO转化为太阳能燃料对于能源可持续性和碳中和具有重要意义。在此，通过碱蚀刻引入的界面重构策略，开发了一种纳米线光催化剂，称为V-BiBrS，其具有丰富的Br和S双空位以及引入了显著近红外（NIR）光响应的表面Bi-O键。所获得的V-BiBrS纳米线在仅在近红外光照射下激发时，表现出将CO转化为CHOH的高效金属光催化还原性能。不含任何助催化剂和牺牲剂，金属缺陷型V-BiBrS的CHOH生成量比BiBrS纳米线高2.3倍。详细的界面结构演变和反应机理已在原子尺度上进行了仔细阐述。这项工作为开发高性能硫基近红外光催化剂提供了独特的界面工程策略，用于将光子还原CO为醇以实现高价值太阳能燃料化学品，这为有效利用延伸至近红外范围的太阳辐射能以实现碳中和目标铺平了道路。
