构建生物炭辅助的 CeO2/g-C3N4 S 型结构,提高光生化 CO2 到 CO 的活性和选择性

IF 5.3 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Materials Research Bulletin Pub Date : 2024-09-07 DOI:10.1016/j.materresbull.2024.113085
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引用次数: 0

摘要

本研究采用多界面接触 S 型光催化剂来还原二氧化碳。利用 g-C3N4 纳米片、氧化 CeO2 纳米颗粒和生物炭(BIO,源自猫尾草)构建了一种混合纳米结构催化剂。g-C3N4-BIO/CeO2 催化剂在气-固-液相二氧化碳还原体系中将二氧化碳转化为一氧化碳时表现出高选择性(95%)。理论和实验证据表明,多界面和界面内电场(IEF)在提高二氧化碳还原过程中的电子转移和氧化还原能力方面起着至关重要的作用。CeO2 中的 Ce4+ 物种能够提供两个电子,从而促进了将 CO2 转化为 CO 的双电子还原过程。此外,CeO2 中的 Ce4+ 可作为电子捕获剂,在捕获电子后可还原为 Ce3+ 离子,从而促进了 CeO2 内部光生载流子的分离过程。原位漫反射红外傅立叶变换光谱(DRIFTS)表明,COOH* 中间体在整个 CO2 光还原为 CO 的过程中起着决定速率的关键作用。这项研究将有助于开发和应用新型环保的生物基 S 型光催化剂。
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Construction of biochar assisted S-scheme of CeO2/g-C3N4 with enhanced photoreduction CO2 to CO activity and selectivity

The multi-interface contacted S-scheme photocatalyst was used for CO2 reduction in this research. A hybrid nanostructures catalyst was constructed using g-C3N4 nanosheet, oxidized CeO2 nanoparticles, and biochar (BIO, cattail-derived). The g-C3N4-BIO/CeO2 catalyst exhibited high selectivity (> 95 %) in converting CO2 to CO in a gas-solid-liquid phase CO2 reduction system. Theoretical and experimental evidence suggests that the multi-interface and interfacial internal electric field (IEF) play a crucial role in enhancing electron transfer and redox ability in CO2 reduction processes. Ce4+ species in CeO2 have the capability to donate two electrons, facilitating the two-electron reduction process involved in the transformation of CO2 to CO. Additionally, Ce4+ in CeO2 acted as an electron trapping agent and could be reduced to Ce3+ ion after trapping electrons, which facilitated the separation process of photogenerated carriers inside CeO2. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) demonstrated that COOH* intermediate played a key role as the rate determining step in the overall CO2 photoreduction to CO. This investigation will contribute to the development and application of new and environmentally friendly BIO-based S-scheme photocatalysts.

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来源期刊
Materials Research Bulletin
Materials Research Bulletin 工程技术-材料科学:综合
CiteScore
9.80
自引率
5.60%
发文量
372
审稿时长
42 days
期刊介绍: Materials Research Bulletin is an international journal reporting high-impact research on processing-structure-property relationships in functional materials and nanomaterials with interesting electronic, magnetic, optical, thermal, mechanical or catalytic properties. Papers purely on thermodynamics or theoretical calculations (e.g., density functional theory) do not fall within the scope of the journal unless they also demonstrate a clear link to physical properties. Topics covered include functional materials (e.g., dielectrics, pyroelectrics, piezoelectrics, ferroelectrics, relaxors, thermoelectrics, etc.); electrochemistry and solid-state ionics (e.g., photovoltaics, batteries, sensors, and fuel cells); nanomaterials, graphene, and nanocomposites; luminescence and photocatalysis; crystal-structure and defect-structure analysis; novel electronics; non-crystalline solids; flexible electronics; protein-material interactions; and polymeric ion-exchange membranes.
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