{"title":"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","authors":"Guoyang Gao, Yuxin Dai, Ying Lin, Houjuan Qi, Zhanhua Huang","doi":"10.1007/s42114-024-01073-4","DOIUrl":null,"url":null,"abstract":"<div><p>The direct conversion of corn stover into high value-added C<sub>1</sub>/C<sub>2</sub> gases using photocatalysis is a challenging and prospective endeavor. In this work, a sulfur/oxygen dual-vacancies CdS/Co<sub>3</sub>O<sub>4</sub> (CdS-S<sub>v</sub>/Co<sub>3</sub>O<sub>4</sub>-O<sub>v</sub>) 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<sub>v</sub>/Co<sub>3</sub>O<sub>4</sub>-O<sub>v</sub> 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, CH<sub>4</sub>, C<sub>2</sub>H<sub>6</sub>, and C<sub>2</sub>H<sub>4</sub> 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 CH<sub>4</sub> 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 C<sub>1</sub>/C<sub>2</sub> gases through the rational design of photocatalysts and reaction systems.</p><h3>Graphical Abstract</h3><p>A sulfur/oxygen dual-vacancies CdS/Co<sub>3</sub>O<sub>4</sub> Z-scheme heterojunction for the one-step photocatalytic conversion of raw corn stover powder into high-value-added C<sub>1</sub>/C<sub>2</sub> gases</p>\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":7220,"journal":{"name":"Advanced Composites and Hybrid Materials","volume":"7 6","pages":""},"PeriodicalIF":23.2000,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"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\",\"authors\":\"Guoyang Gao, Yuxin Dai, Ying Lin, Houjuan Qi, Zhanhua Huang\",\"doi\":\"10.1007/s42114-024-01073-4\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The direct conversion of corn stover into high value-added C<sub>1</sub>/C<sub>2</sub> gases using photocatalysis is a challenging and prospective endeavor. In this work, a sulfur/oxygen dual-vacancies CdS/Co<sub>3</sub>O<sub>4</sub> (CdS-S<sub>v</sub>/Co<sub>3</sub>O<sub>4</sub>-O<sub>v</sub>) 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<sub>v</sub>/Co<sub>3</sub>O<sub>4</sub>-O<sub>v</sub> 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, CH<sub>4</sub>, C<sub>2</sub>H<sub>6</sub>, and C<sub>2</sub>H<sub>4</sub> 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 CH<sub>4</sub> 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 C<sub>1</sub>/C<sub>2</sub> gases through the rational design of photocatalysts and reaction systems.</p><h3>Graphical Abstract</h3><p>A sulfur/oxygen dual-vacancies CdS/Co<sub>3</sub>O<sub>4</sub> Z-scheme heterojunction for the one-step photocatalytic conversion of raw corn stover powder into high-value-added C<sub>1</sub>/C<sub>2</sub> gases</p>\\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":7220,\"journal\":{\"name\":\"Advanced Composites and Hybrid Materials\",\"volume\":\"7 6\",\"pages\":\"\"},\"PeriodicalIF\":23.2000,\"publicationDate\":\"2024-11-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Advanced Composites and Hybrid Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s42114-024-01073-4\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, COMPOSITES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Composites and Hybrid Materials","FirstCategoryId":"88","ListUrlMain":"https://link.springer.com/article/10.1007/s42114-024-01073-4","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, COMPOSITES","Score":null,"Total":0}
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
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-Sv/Co3O4-Ov) 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-Sv/Co3O4-Ov 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
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.