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Light-Mediated Sustainable Conversion of Carbon Dioxide to Valuable Methanol by Highly Efficient Covalent Organic Framework g-C3N4 Composites as a Reusable Photocatalyst
Industrial & Engineering Chemistry Research ( IF 4.2 ) Pub Date : 2024-03-25 , DOI: 10.1021/acs.iecr.3c03572
Mainak Sarkar 1 , Pekham Chakrabortty 1 , Manideepa Sengupta 1 , Anil Chandra Kothari 2, 3 , Mohammad Shahidul Islam 4 , Sk. Manirul Islam 1
Affiliation  

A novel triazine-based structured two-dimensional (2D) covalent organic framework (COF), known as TRITER-1, has been prepared through the Schiff-base condensation reaction between terephthalaldehyde and 1,3,5-tris(4-aminophenyl)triazine. Additionally, g-C3N4 has been incorporated within imine-based covalent organic frameworks to produce the composite known as TRITER-1@g-C3N4, which has a relatively small band gap of 2.0 eV. This composite, called TRITER-1@g-C3N4, has been synthesized and effectively used toward the light-driven formation of methanol from the most greenhouse gas CO2. This highly crystalline organic polymeric material demonstrated an outstanding photocatalytic activity. The active photocatalyst TRITER-1@g-C3N4 composite successfully reduces CO2 into methanol under ambient reaction conditions in the presence of NiO nanoparticles as a cocatalyst under atmospheric pressure. The visible-light-accelerated metal-free CO2 reduction into methanol by this COF composite has been accomplished under 15 W of a white LED light illumination, with a maximum turnover number of (TON = 172, μmol = 22 600). By varying the light intensity, it was clear that the reaction failed to take place in the absence of a white LED. We proved that sunlight can also produce a TON of around 73 under conditions that allow for sustainable reactions. This catalyst retains its catalytic function after being regenerated multiple times and is effective and selective.

中文翻译:

高效共价有机骨架 g-C3N4 复合材料作为可重复使用的光催化剂,在光介导下将二氧化碳可持续转化为有价值的甲醇

通过对苯二甲醛和1,3,5-三(4-氨基苯基)之间的希夫碱缩合反应制备了一种新型三嗪基结构二维(2D)共价有机骨架(COF),称为TRITER-1三嗪。此外,gC 3 N 4已被纳入基于亚胺的共价有机骨架中,以产生称为TRITER-1@gC 3 N 4的复合材料,其具有相对较小的带隙(2.0 eV)。这种复合材料被称为 TRITER-1@gC 3 N 4,已被合成并有效地用于光驱动从大多数温室气体 CO 2中形成甲醇。这种高度结晶的有机聚合物材料表现出出色的光催化活性。活性光催化剂TRITER-1@gC 3 N 4复合材料在大气压力下,在NiO纳米颗粒作为助催化剂的存在下,在环境反应条件下成功地将CO 2还原为甲醇。该COF复合材料在15 W白光LED光照射下实现了可见光加速的无金属CO 2还原为甲醇,最大周转数为(TON = 172,μmol = 22 600)。通过改变光强度,很明显,在没有白色 LED 的情况下,反应无法发生。我们证明,在允许可持续反应的条件下,阳光也可以产生约 73 TON 的能量。该催化剂经多次再生后仍能保持其催化功能,且具有高效性和选择性。
更新日期:2024-03-25
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