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光催化Nat. Commun：富范德华间隙的二维超薄BiOCl在纯水体系高效光催化还原CO2制CO
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上海交通大学张礼知教授（杰青、长江、万人计划领军人才，https://sese.sjtu.edu.cn/faculty/view/117）携手其博士弟子李杰（现为河南大学第四层次特聘教授https://phye.henu.edu.cn/info/1069/4394.htm）、石彦彪（上海交通大学博后）、毛成梁（多伦多大学博后），与大连化物所黄延强研究员（杰青）合作，在nature communications发表了题为“van der waals gap-rich biocl atomic layers realizing efficient, pure-water co2-to-co photocatalysis”研究论文。 该研究开发出一种高效的光催化还原二氧化碳工艺，在仅使用可见光、纯水、co2和原子级富含范德华间隙的biocl纳米片的情况下，高效通过光催化co2还原制备co。该biocl纳米片的合成是通过与合成气合成路线类似的气相剥离策略实现的，其具有石墨烯模拟结构，基面由范德华间隙包裹。这种高范德华间隙覆盖率(99%)会赋予纳米片在性能上的两个关键优势，即超低的激子结合能和高催化活性vdwg-bi-vo••-bi位点。这些优点促进了激子至电子与co2至co的转化，从而使纯水pcr的速率达到188.2 μmol g−1 h−1。此前对层状材料的研究主要集中在剥离以获得超薄原子层(但范德华间隙覆盖率较低)、缺陷工程以创建活性位点、以及掺杂和单原子负载以活化共价键合面中；与之相比，本研究开发的vdwg工程策略有可能为层状光催化剂的性能最大化增加一个维度。 文章链接 https://www.nature.com/articles/s41467-021-26219-6 期刊 nature communications doi 10.1038/s41467-021-26219-6 题目 van der waals gap-rich biocl atomic layers realizing efficient, pure-water co2-to-co photocatalysis 作者 yanbiao shi, jie li, chengliang mao, song liu, xiaobing wang, xiufan liu, shengxi zhao, xiao liu, yanqiang huang & lizhi zhang 摘要 photocatalytic co2 reduction (pcr) is able to convert solar energy into chemicals, fuels, and feedstocks, but limited by the deficiencies of photocatalysts in steering photon-to-electron conversion and activating co2, especially in pure water. here we report an efficient, pure water co2-to-co conversion photocatalyzed by sub-3-nm-thick biocl nanosheets with van der waals gaps (vdwgs) on the two-dimensional facets, a graphene-analog motif distinct from the majority of previously reported nanosheets usually bearing vdwgs on the lateral facets. compared with bulk biocl, the vdwgs-rich atomic layers possess a weaker excitonic confinement power to decrease exciton binding energy from 137 to 36 mev, consequently yielding a 50-fold enhancement in the bulk charge separation efficiency. moreover, the vdwgs facilitate the formation of vdwg-bi-vo••-bi defect, a highly active site to accelerate the co2-to-co transformation via the synchronous optimization of co2 activation, *cooh splitting, and *co desorption. the improvements in both exciton-to-electron and co2-to-co conversions result in a visible light pcr rate of 188.2 μmol g−1 h−1 in pure water without any co-catalysts, hole scavengers, or organic solvents. these results suggest that increasing vdwg exposure is a way for designing high-performance solar-fuel generation systems.  2021-10-13_165232.jpg  2021-10-13_165949.jpg  2021-10-13_170009.jpg  2021-10-13_170043.jpg  2021-10-13_170055.jpg |
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