Li Siru, Tian Yu, Yan Likai, Su Zhongmin
Institute of Functional Material Chemistry, National & Local United Engineering Lab for Power Battery, Key Laboratory of Polyoxometalate Science of Ministry of Education, Faculty of Chemistry, Northeast Normal University, Changchun 130024, P. R. China.
Phys Chem Chem Phys. 2021 Feb 7;23(5):3401-3406. doi: 10.1039/d0cp05713d. Epub 2021 Jan 28.
Photocatalytic reduction of CO to hydrocarbons is considered to be a promising strategy to solve the energy crisis and environmental problems. Herein, the electronic and optical properties, and catalytic performance of g-CN derivatives [CN(CH)] (systems 1 and 2), and [CN(CH)] (system 3) were studied by density functional theory (DFT) computations. Compared to g-CN the band gaps of systems 1-3 are smaller, and the absorption intensities of the three derivatives in the visible light region increase, indicating that these derivatives can produce more electrons under visible light irradiation and enhance the photocatalytic performance. The computational results show that the main products of CO reduction catalyzed by system 1 are HCOOH and CHOH. The rate-determining step is CO→ COOH* with a ΔG of 1.22 eV. Therefore, system 1 is predicted to be a promising catalyst for the CO reduction reaction.
光催化将CO还原为碳氢化合物被认为是解决能源危机和环境问题的一种有前景的策略。在此，通过密度泛函理论（DFT）计算研究了g-CN衍生物[CN(CH)]（体系1和2）以及[CN(CH)]（体系3）的电子和光学性质及催化性能。与g-CN相比，体系1-3的带隙更小，且这三种衍生物在可见光区域的吸收强度增加，表明这些衍生物在可见光照射下能产生更多电子并增强光催化性能。计算结果表明，体系1催化CO还原的主要产物是HCOOH和CHOH。速率决定步骤是CO→COOH*，ΔG为1.22 eV。因此，体系1被预测为一种有前景的CO还原反应催化剂。
