An innovative CuxAg50−x/UiO66-NH2 photocatalyst prepared using a dual ship bottling strategy for photocatalytic CO2 reduction: controlled product selectivity and pathways
{"title":"An innovative CuxAg50−x/UiO66-NH2 photocatalyst prepared using a dual ship bottling strategy for photocatalytic CO2 reduction: controlled product selectivity and pathways","authors":"Lipeng Jiang, Dengqian Chen, Zhengkai Hao, Dongxue Cao, Runqiao Liu, Jingyu Cheng, Limei Chen, Xin Liu, Boyin Jia, Dongdong Liu","doi":"10.1039/d4ee03103b","DOIUrl":null,"url":null,"abstract":"Photocatalytic CO<small><sub>2</sub></small> reduction technology is one of the most promising solutions to solve the greenhouse effect and global energy crisis. However, its low conversion efficiency and poor product selectivity greatly limit the practical application of this technology. This study innovatively proposed a “dual ship bottling” strategy to prepare a Cu<small><sub><em>x</em></sub></small>Ag<small><sub>50−<em>x</em></sub></small>/UiO66-NH<small><sub>2</sub></small> catalyst for the photocatalytic CO<small><sub>2</sub></small> reduction reaction (CO<small><sub>2</sub></small>RR). Many individual Cu<small><sub><em>x</em></sub></small>Ag<small><sub>50−<em>x</em></sub></small> alloys were successfully encapsulated within UiO66-NH<small><sub>2</sub></small>, and the nano-confinement effect of UiO66-NH<small><sub>2</sub></small> effectively prevented the aggregation of Cu<small><sub><em>x</em></sub></small>Ag<small><sub>50−<em>x</em></sub></small> alloys, thereby significantly improving the catalytic activity of Cu<small><sub><em>x</em></sub></small>Ag<small><sub>50−<em>x</em></sub></small>/UiO66-NH<small><sub>2</sub></small>. The Cu<small><sub><em>x</em></sub></small>Ag<small><sub>50−<em>x</em></sub></small>/UiO66-NH<small><sub>2</sub></small> photocatalytic system with different Cu : Ag molar ratios exhibited astonishing yields (38.64–162.47 μmol g<small><sup>−1</sup></small> h<small><sup>−1</sup></small>) of reduced carbon products, excellent cycling stability and long-term durability exceeding 30 h, as well as the corresponding selectivity for C<small><sub>2</sub></small>–(C<small><sub>2</sub></small>H<small><sub>4</sub></small>, C<small><sub>2</sub></small>H<small><sub>5</sub></small>OH), C<small><sub>1</sub></small>–(CH<small><sub>4</sub></small>, CH<small><sub>3</sub></small>OH), C<small><sub>1</sub></small>–(CO) was 91.67%, 96.25% and 93.01%, respectively. Under visible light irradiation, some photogenerated electrons were transferred from UiO66-NH<small><sub>2</sub></small> to Cu<small><sub><em>x</em></sub></small>Ag<small><sub>50−<em>x</em></sub></small> alloys. The different bonding strengths between Cu–Ag catalytic active sites in Cu<small><sub><em>x</em></sub></small>Ag<small><sub>50−<em>x</em></sub></small> alloys and *CO intermediates determined the three subsequent reaction pathways of *CO (*CO → α, α = *COCO, *CHO and CO). In addition, Cu<small><sub><em>x</em></sub></small>Ag<small><sub>50−<em>x</em></sub></small>/UiO66-NH<small><sub>2</sub></small> exhibited strong adsorption of *H intermediates, effectively inhibiting the hydrogen evolution reaction (HER). Finally, the regulation mechanism of Cu<small><sub><em>x</em></sub></small>Ag<small><sub>50−<em>x</em></sub></small>/UiO66-NH<small><sub>2</sub></small> for the photocatalytic CO<small><sub>2</sub></small>RR was revealed. This study provides a new insight into the design of new photocatalysts and selective regulation of reduced carbon products.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":null,"pages":null},"PeriodicalIF":32.4000,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Energy & Environmental Science","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1039/d4ee03103b","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Photocatalytic CO2 reduction technology is one of the most promising solutions to solve the greenhouse effect and global energy crisis. However, its low conversion efficiency and poor product selectivity greatly limit the practical application of this technology. This study innovatively proposed a “dual ship bottling” strategy to prepare a CuxAg50−x/UiO66-NH2 catalyst for the photocatalytic CO2 reduction reaction (CO2RR). Many individual CuxAg50−x alloys were successfully encapsulated within UiO66-NH2, and the nano-confinement effect of UiO66-NH2 effectively prevented the aggregation of CuxAg50−x alloys, thereby significantly improving the catalytic activity of CuxAg50−x/UiO66-NH2. The CuxAg50−x/UiO66-NH2 photocatalytic system with different Cu : Ag molar ratios exhibited astonishing yields (38.64–162.47 μmol g−1 h−1) of reduced carbon products, excellent cycling stability and long-term durability exceeding 30 h, as well as the corresponding selectivity for C2–(C2H4, C2H5OH), C1–(CH4, CH3OH), C1–(CO) was 91.67%, 96.25% and 93.01%, respectively. Under visible light irradiation, some photogenerated electrons were transferred from UiO66-NH2 to CuxAg50−x alloys. The different bonding strengths between Cu–Ag catalytic active sites in CuxAg50−x alloys and *CO intermediates determined the three subsequent reaction pathways of *CO (*CO → α, α = *COCO, *CHO and CO). In addition, CuxAg50−x/UiO66-NH2 exhibited strong adsorption of *H intermediates, effectively inhibiting the hydrogen evolution reaction (HER). Finally, the regulation mechanism of CuxAg50−x/UiO66-NH2 for the photocatalytic CO2RR was revealed. This study provides a new insight into the design of new photocatalysts and selective regulation of reduced carbon products.
期刊介绍:
Energy & Environmental Science, a peer-reviewed scientific journal, publishes original research and review articles covering interdisciplinary topics in the (bio)chemical and (bio)physical sciences, as well as chemical engineering disciplines. Published monthly by the Royal Society of Chemistry (RSC), a not-for-profit publisher, Energy & Environmental Science is recognized as a leading journal. It boasts an impressive impact factor of 8.500 as of 2009, ranking 8th among 140 journals in the category "Chemistry, Multidisciplinary," second among 71 journals in "Energy & Fuels," second among 128 journals in "Engineering, Chemical," and first among 181 scientific journals in "Environmental Sciences."
Energy & Environmental Science publishes various types of articles, including Research Papers (original scientific work), Review Articles, Perspectives, and Minireviews (feature review-type articles of broad interest), Communications (original scientific work of an urgent nature), Opinions (personal, often speculative viewpoints or hypotheses on current topics), and Analysis Articles (in-depth examination of energy-related issues).