Hayat Asif, Shaishta Naghma, Uddin Ikram, Khan Muhammad, Mane Sunil Kumar Baburao, Hayat Ashiq, Ullah Ikram, Ur Rehman Ata, Ali Tariq, Manjunatha G
State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou 350002, PR China.
Department of Post-Graduate Studies and Research in Chemistry, Gulbarga University, Gulbarga 585106, India.
J Colloid Interface Sci. 2021 Sep;597:39-47. doi: 10.1016/j.jcis.2021.03.159. Epub 2021 Mar 31.
The development of superior heterogeneous catalyst for hydrogen (H) evolution is a significant feature and challenging for determining the energy and environmental crises. However, the dumping of numerous lethal colorants (dye) as of textile manufacturing has fascinated widespread devotion-aimed water pollution anticipation and treatment. In this regard, a photocatalytic H evolution by visible light using low-dimensional semiconducting materials having pollutant degradable capacity for Rhodamine B dyes (RhB) has been anticipated as a route towards environmental aspect. Here we fabricated the incorporation of organic electron-rich heterocyclic monomer 2,6-dimethylmorpholine (MP), inside electron-poor graphitic carbon nitride (g-CN) semiconductor by solid-state co-polymerization. The supremacy of copolymerization process was successfully examined via absorbent, calculated band gap, and migration of electrons on the photocatalytic performance of as-constructed CN-MP copolymer. The density functional theory (DFT) calculation provides extra support as evident for the successful integration of MP into the g-CN framework by this means-reduced band gap upon co-polymerization. The hydrogen evolution rate (HER) for g-CN was found as 115.2 μmol/h, whereas for CN-PMwas estimated at 641.2 μmol/h (six times higher). In particular, the pseudo-order kinetic constant of CN-MP for photodegradation of RhB was two times higher than that ofg-CN. Results show an important step toward tailor-designed and explain the vital role of the D-A system for the rational motifs of productive photocatalysts with effective pollutant degradable capability for future demand.
开发用于析氢的优质非均相催化剂是解决能源和环境危机的一个重要特征且具有挑战性。然而，纺织制造业排放的大量致命染料引发了广泛致力于水污染预防和治理的关注。在这方面，利用对罗丹明B染料（RhB）具有污染物降解能力的低维半导体材料通过可见光进行光催化析氢被视为实现环境目标的一条途径。在此，我们通过固态共聚法将富电子有机杂环单体2,6 - 二甲基吗啉（MP）引入到缺电子的石墨相氮化碳（g - CN）半导体中。通过吸收光谱、计算带隙以及电子迁移对所构建的CN - MP共聚物的光催化性能成功检验了共聚过程的优越性。密度泛函理论（DFT）计算提供了额外支持，证明通过这种方式MP成功整合到g - CN框架中——共聚时带隙减小。发现g - CN的析氢速率（HER）为115.2 μmol/h，而CN - PM的析氢速率估计为641.2 μmol/h（高出六倍）。特别地，CN - MP对RhB光降解的准一级动力学常数是g - CN的两倍。结果显示了朝着定制设计迈出的重要一步，并解释了给体 - 受体（D - A）体系对于具有有效污染物降解能力以满足未来需求的高效光催化剂合理设计的关键作用。
