Efficient charge separation in Z-scheme heterojunctions induced by chemical bonding-enhanced internal electric field for promoting photocatalytic conversion of corn stover to C1/C2 gases

IF 23.2 2区材料科学 Q1 MATERIALS SCIENCE, COMPOSITES Advanced Composites and Hybrid Materials Pub Date : 2024-11-19 DOI:10.1007/s42114-024-01073-4

Guoyang Gao, Yuxin Dai, Ying Lin, Houjuan Qi, Zhanhua Huang

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Abstract

The direct conversion of corn stover into high value-added C₁/C₂ gases using photocatalysis is a challenging and prospective endeavor. In this work, a sulfur/oxygen dual-vacancies CdS/Co₃O₄ (CdS-S_v/Co₃O₄-O_v) Z-scheme heterojunction was designed for direct raw corn stover powder (RCSP) conversion in a photoreactive system. The internal electric field (IEF) formed in CdS-S_v/Co₃O₄-O_v can effectively promote the photogenerated charge separation and transfer, and the chemical bond formed at the heterogeneous interface can be used as a channel for the directional migration of photogenerated charges to accelerate the inter-interface charge transfer. Experimental results combined with DFT calculations confirmed the formation of Z-scheme heterojunction and IEF. The results of the photocatalytic RCSP reaction showed that the CO, CH₄, C₂H₆, and C₂H₄ evolution rates of the proposed catalytic system were as high as 691.99, 2057.69, 202.93, and 187.29 µmol/g, with the corresponding CH₄ selectivity and total hydrocarbon selectivity of 65.53% and 77.96%, respectively. What is more, we propose a photocatalytic reaction mechanism in which raw biomass undergoes depolymerization and cascading oxidation to high value-added products. This study provides a new idea for high-performance photocatalytic direct conversion of RCSP into high-value-added C₁/C₂ gases through the rational design of photocatalysts and reaction systems.

Graphical Abstract

A sulfur/oxygen dual-vacancies CdS/Co₃O₄ Z-scheme heterojunction for the one-step photocatalytic conversion of raw corn stover powder into high-value-added C₁/C₂ gases

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化学键增强内电场诱导 Z 型异质结中的高效电荷分离，促进玉米秸秆向 C1/C2 气体的光催化转化

利用光催化将玉米秸秆直接转化为高附加值的 C1/C2 气体是一项具有挑战性和前瞻性的工作。本研究设计了一种硫/氧双空位 CdS/Co3O4（CdS-Sv/Co3O4-Ov）Z 型异质结，用于在光活性体系中直接转化生玉米秸秆粉（RCSP）。CdS-Sv/Co3O4-Ov 中形成的内电场（IEF）可有效促进光生电荷的分离和转移，而异质界面上形成的化学键可作为光生电荷定向迁移的通道，从而加速界面间的电荷转移。实验结果结合 DFT 计算证实了 Z 型异质结和 IEF 的形成。光催化 RCSP 反应的结果表明，该催化体系的 CO、CH4、C2H6 和 C2H4 进化速率分别高达 691.99、2057.69、202.93 和 187.29 µmol/g，相应的 CH4 选择性和总烃选择性分别为 65.53% 和 77.96%。此外，我们还提出了一种光催化反应机理，即生物质原料经过解聚和级联氧化反应生成高附加值产品。本研究通过合理设计光催化剂和反应体系，为高性能光催化将 RCSP 直接转化为高附加值的 C1/C2 气体提供了新思路。图文并茂的摘要一种硫氧双空位 CdS/Co3O4 Z 型异质结用于一步法光催化将玉米秸秆原料粉转化为高附加值的 C1/C2 气体

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来源期刊

Advanced Composites and Hybrid Materials Multiple-

CiteScore

26.00

自引率

21.40%

发文量

185

期刊介绍： Advanced Composites and Hybrid Materials is a leading international journal that promotes interdisciplinary collaboration among materials scientists, engineers, chemists, biologists, and physicists working on composites, including nanocomposites. Our aim is to facilitate rapid scientific communication in this field. The journal publishes high-quality research on various aspects of composite materials, including materials design, surface and interface science/engineering, manufacturing, structure control, property design, device fabrication, and other applications. We also welcome simulation and modeling studies that are relevant to composites. Additionally, papers focusing on the relationship between fillers and the matrix are of particular interest. Our scope includes polymer, metal, and ceramic matrices, with a special emphasis on reviews and meta-analyses related to materials selection. We cover a wide range of topics, including transport properties, strategies for controlling interfaces and composition distribution, bottom-up assembly of nanocomposites, highly porous and high-density composites, electronic structure design, materials synergisms, and thermoelectric materials. Advanced Composites and Hybrid Materials follows a rigorous single-blind peer-review process to ensure the quality and integrity of the published work.