The Reduced Barrier for the Photogenerated Charge Migration on Covalent Triazine-Based Frameworks for Boosting Photocatalytic CO2 Reduction Into Syngas

IF 5.1 Q1 POLYMER SCIENCE ACS Macro Letters Pub Date : 2024-11-13 DOI:10.1002/adfm.202417109
Ke Kong, Hong Zhong, Fushuai Zhang, Haowei Lv, Xiaoju Li, Ruihu Wang
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Abstract

Photocatalytic CO2 reduction together with hydrogen generation is a promising approach to generate syngas, the photogenerated electron migration from photosensitizers to the catalytic active sites is the rate-determining step. Herein, an integrative strategy is presented by covalently grafting metal complexes into donor–acceptor covalent triazine-based frameworks. The catalytic active sites are integrated with the photosensitizer units by covalent linkages to form an extended π-conjugated framework, which significantly reduces the energy barrier for the migration of the photogenerated charge carriers, resulting in high activity and durability in photocatalytic CO2 reduction into syngas under visible light irradiation. The CO and H2 evolution amounts in 1.5 h are 1086 and 1042 µmol g−1, respectively, which greatly surpass those in the host-guest counterparts. Furthermore, selective adsorption for CO2 over N2 renders this photocatalytic system to be effective for syngas production from the simulated flue gas. This study provides new approaches to construct the integrative photocatalytic systems for solar-to-chemical energy conversion.

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降低共价三嗪基框架上光生电荷迁移的障碍,促进光催化二氧化碳还原为合成气
光催化二氧化碳还原和制氢是产生合成气的一种可行方法,光敏剂产生的电子迁移到催化活性位点是决定速率的步骤。本文提出了一种综合策略,将金属复合物共价接枝到供体-受体共价三嗪基框架中。催化活性位点通过共价连接与光敏剂单元结合在一起,形成一个扩展的π-共轭框架,从而大大降低了光生电荷载流子迁移的能量势垒,使光催化二氧化碳还原成合成气的过程在可见光照射下具有高活性和持久性。在 1.5 小时内,CO 和 H2 的进化量分别为 1086 微摩尔 g-1 和 1042 微摩尔 g-1,大大超过了主客体对应物的进化量。此外,光催化系统对 CO2 的选择性吸附超过了对 N2 的选择性吸附,使其能有效地从模拟烟气中产生合成气。这项研究为构建太阳能到化学能转换的集成光催化系统提供了新方法。
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来源期刊
CiteScore
10.40
自引率
3.40%
发文量
209
审稿时长
1 months
期刊介绍: ACS Macro Letters publishes research in all areas of contemporary soft matter science in which macromolecules play a key role, including nanotechnology, self-assembly, supramolecular chemistry, biomaterials, energy generation and storage, and renewable/sustainable materials. Submissions to ACS Macro Letters should justify clearly the rapid disclosure of the key elements of the study. The scope of the journal includes high-impact research of broad interest in all areas of polymer science and engineering, including cross-disciplinary research that interfaces with polymer science. With the launch of ACS Macro Letters, all Communications that were formerly published in Macromolecules and Biomacromolecules will be published as Letters in ACS Macro Letters.
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