{"title":"金属- salen - incorporated共轭微孔聚合物作为太阳能驱动的大气CO2与H2O还原的坚固人工叶片","authors":"Wei Wu, Zhaocen Dong, Mantao Chen, Waner Li, An Liao, Qing Liu, Yachao Zhang, Zhixin Zhou, Chao Zeng, Xuezhong Gong, Chunhui Dai","doi":"10.1002/cey2.646","DOIUrl":null,"url":null,"abstract":"<p>Exploration of efficient and stable photocatalysts to mimic natural leaves for the conversion of atmospheric CO<sub>2</sub> into hydrocarbons utilizing solar light is very important but remains a major challenge. Herein, we report the design of four novel metal–salen-incorporated conjugated microporous polymers as robust artificial leaves for photoreduction of atmospheric CO<sub>2</sub> with gaseous water. Owing to the rich nitrogen and oxygen moieties in the polymeric frameworks, they show a maximum CO<sub>2</sub> adsorption capacity of 46.1 cm<sup>3</sup> g<sup>−1</sup> and adsorption selectivity for CO<sub>2</sub>/N<sub>2</sub> of up to 82 at 273 K. Under air atmosphere and simulated solar light (100 mW cm<sup>−2</sup>), TEPT-Zn shows an excellent CO yield of 304.96 μmol h<sup>−1</sup> g<sup>−1</sup> with a selectivity of approximately 100%, which represents one of the best results in terms of organic photocatalysts for gas-phase CO<sub>2</sub> photoreduction so far. Furthermore, only small degradation in the CO yield is observed even after 120-h continuous illumination. More importantly, a good CO yield of 152.52 μmol g<sup>−1</sup> was achieved by directly exposing the photocatalytic reaction of TEPT-Zn in an outdoor environment for 3 h (25–28°C, 52.3 ± 7.9 mW cm<sup>−2</sup>). This work provides an avenue for the continued development of advanced polymers toward gas-phase photoconversion of CO<sub>2</sub> from air.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 1","pages":""},"PeriodicalIF":19.5000,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.646","citationCount":"0","resultStr":"{\"title\":\"Metal–Salen-Incorporated conjugated microporous polymers as robust artificial leaves for solar-driven reduction of atmospheric CO2 with H2O\",\"authors\":\"Wei Wu, Zhaocen Dong, Mantao Chen, Waner Li, An Liao, Qing Liu, Yachao Zhang, Zhixin Zhou, Chao Zeng, Xuezhong Gong, Chunhui Dai\",\"doi\":\"10.1002/cey2.646\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Exploration of efficient and stable photocatalysts to mimic natural leaves for the conversion of atmospheric CO<sub>2</sub> into hydrocarbons utilizing solar light is very important but remains a major challenge. Herein, we report the design of four novel metal–salen-incorporated conjugated microporous polymers as robust artificial leaves for photoreduction of atmospheric CO<sub>2</sub> with gaseous water. Owing to the rich nitrogen and oxygen moieties in the polymeric frameworks, they show a maximum CO<sub>2</sub> adsorption capacity of 46.1 cm<sup>3</sup> g<sup>−1</sup> and adsorption selectivity for CO<sub>2</sub>/N<sub>2</sub> of up to 82 at 273 K. Under air atmosphere and simulated solar light (100 mW cm<sup>−2</sup>), TEPT-Zn shows an excellent CO yield of 304.96 μmol h<sup>−1</sup> g<sup>−1</sup> with a selectivity of approximately 100%, which represents one of the best results in terms of organic photocatalysts for gas-phase CO<sub>2</sub> photoreduction so far. Furthermore, only small degradation in the CO yield is observed even after 120-h continuous illumination. 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引用次数: 0
摘要
探索高效和稳定的光催化剂来模拟自然树叶利用太阳光将大气中的二氧化碳转化为碳氢化合物是非常重要的,但仍然是一个主要的挑战。在这里,我们报道了四种新型金属-盐结合的共轭微孔聚合物的设计,作为大气CO2与气态水的光还原的坚固人工叶子。由于聚合物框架中含有丰富的氮和氧基团,在273 K下,它们对CO2的最大吸附量为46.1 cm3 g−1,对CO2/N2的吸附选择性高达82。在空气气氛和模拟太阳光(100 mW cm−2)下,TEPT-Zn的CO产率为304.96 μmol h−1 g−1,选择性约为100%,是目前气相CO2光还原效果最好的有机光催化剂之一。此外,即使在连续照明120小时后,CO产率也只有很小的下降。更重要的是,将TEPT-Zn光催化反应在室外环境(25-28°C, 52.3±7.9 mW cm - 2)中直接暴露3 h, CO产率达到152.52 μmol g - 1。这项工作为继续开发先进的聚合物以实现空气中CO2的气相光转化提供了一条途径。
Metal–Salen-Incorporated conjugated microporous polymers as robust artificial leaves for solar-driven reduction of atmospheric CO2 with H2O
Exploration of efficient and stable photocatalysts to mimic natural leaves for the conversion of atmospheric CO2 into hydrocarbons utilizing solar light is very important but remains a major challenge. Herein, we report the design of four novel metal–salen-incorporated conjugated microporous polymers as robust artificial leaves for photoreduction of atmospheric CO2 with gaseous water. Owing to the rich nitrogen and oxygen moieties in the polymeric frameworks, they show a maximum CO2 adsorption capacity of 46.1 cm3 g−1 and adsorption selectivity for CO2/N2 of up to 82 at 273 K. Under air atmosphere and simulated solar light (100 mW cm−2), TEPT-Zn shows an excellent CO yield of 304.96 μmol h−1 g−1 with a selectivity of approximately 100%, which represents one of the best results in terms of organic photocatalysts for gas-phase CO2 photoreduction so far. Furthermore, only small degradation in the CO yield is observed even after 120-h continuous illumination. More importantly, a good CO yield of 152.52 μmol g−1 was achieved by directly exposing the photocatalytic reaction of TEPT-Zn in an outdoor environment for 3 h (25–28°C, 52.3 ± 7.9 mW cm−2). This work provides an avenue for the continued development of advanced polymers toward gas-phase photoconversion of CO2 from air.
期刊介绍:
Carbon Energy is an international journal that focuses on cutting-edge energy technology involving carbon utilization and carbon emission control. It provides a platform for researchers to communicate their findings and critical opinions and aims to bring together the communities of advanced material and energy. The journal covers a broad range of energy technologies, including energy storage, photocatalysis, electrocatalysis, photoelectrocatalysis, and thermocatalysis. It covers all forms of energy, from conventional electric and thermal energy to those that catalyze chemical and biological transformations. Additionally, Carbon Energy promotes new technologies for controlling carbon emissions and the green production of carbon materials. The journal welcomes innovative interdisciplinary research with wide impact. It is indexed in various databases, including Advanced Technologies & Aerospace Collection/Database, Biological Science Collection/Database, CAS, DOAJ, Environmental Science Collection/Database, Web of Science and Technology Collection.