Long Yang, Ramesh Poonchi Sivasankaran, Mee Kyung Song, Amol Uttam Pawar, Don Keun Lee, Young Soo Kang
{"title":"Highly Selective Solar CO2 Conversion into Formic Acid in Nickel-Perylene-C3N4 Semiconductor Photocatalyst","authors":"Long Yang, Ramesh Poonchi Sivasankaran, Mee Kyung Song, Amol Uttam Pawar, Don Keun Lee, Young Soo Kang","doi":"10.1002/aenm.202402798","DOIUrl":null,"url":null,"abstract":"Photocatalytic (PC) CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) into value-added oxygenated products is one of the most promising ways of solving climate warming change and energy crisis simultaneously. To reach higher selectivity and productivity of fuel products, it still remains great challenge in controlling both simultaneous sequential multi-electron/proton shuttling through different transporting pathway, which determines the intermediates and final products. Consequently, a multifunctional nickel-perylene-carbon nitride nanosheet (NS-P-g-C<sub>3</sub>N<sub>4</sub>-Ni) are constructed rationally to strengthen the electron and proton transfer via different pathway at the same time through molecule-level carbon backbone with excellent conductivity/charge capacity and proton transport via pendant functional group of -NH<sub>2</sub> from water oxidation sites of Ni metal cluster on perylene skeleton. CO<sub>2</sub> adsorption is enhanced and reduction energy is reduced by the complexation of N-atom site of NS-P-g-C<sub>3</sub>N<sub>4</sub>-Ni and adjustment of co-planarity, optimizing conduction band and band gap with energy controllable techniques. In situ FT-IR/Raman/EPR spectra identified and verified the transformation of active intermediates (<sup>*</sup>CO<sub>2</sub><sup>•−</sup>, <sup>*</sup>COOH and H<sup>*</sup>COO<sup>−</sup>) adsorbed on the NS-P-g-C<sub>3</sub>N<sub>4</sub>-Ni by complexation and highly selective production of formic acid (60%) is achieved. This work sheds light on the construction of effective well-structured sites in photocatalytic CO<sub>2</sub> reduction to produce value-added products with higher selectivity and productivity.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":24.4000,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Energy Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/aenm.202402798","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Photocatalytic (PC) CO2 reduction reaction (CO2RR) into value-added oxygenated products is one of the most promising ways of solving climate warming change and energy crisis simultaneously. To reach higher selectivity and productivity of fuel products, it still remains great challenge in controlling both simultaneous sequential multi-electron/proton shuttling through different transporting pathway, which determines the intermediates and final products. Consequently, a multifunctional nickel-perylene-carbon nitride nanosheet (NS-P-g-C3N4-Ni) are constructed rationally to strengthen the electron and proton transfer via different pathway at the same time through molecule-level carbon backbone with excellent conductivity/charge capacity and proton transport via pendant functional group of -NH2 from water oxidation sites of Ni metal cluster on perylene skeleton. CO2 adsorption is enhanced and reduction energy is reduced by the complexation of N-atom site of NS-P-g-C3N4-Ni and adjustment of co-planarity, optimizing conduction band and band gap with energy controllable techniques. In situ FT-IR/Raman/EPR spectra identified and verified the transformation of active intermediates (*CO2•−, *COOH and H*COO−) adsorbed on the NS-P-g-C3N4-Ni by complexation and highly selective production of formic acid (60%) is achieved. This work sheds light on the construction of effective well-structured sites in photocatalytic CO2 reduction to produce value-added products with higher selectivity and productivity.
期刊介绍:
Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small.
With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics.
The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.