Solar-induced photothermal catalysis of CO₂ reduction is an effective method for chemical CO₂ conversion with great potential. Understanding its reaction mechanism is crucial for the development of new catalysts. In this work, the mechanism of CO₂ reduction on a BaTiO₃ supported Ni catalyst was studied using density functional theory (DFT). The presence of the BaTiO₃ base was found to have great significance in the adsorption and activation of CO₂. The dominant reaction pathway of CO₂ reduction on the BaTiO₃ supported Ni catalyst is calculated as CO₂(g)→CO₂→CO→COH→HCOH→CH→CH₂→CH₃→CH₄→CH₄(g) and is rate-limited by the reduction of CO, with a corresponding energy barrier of 0.94 eV, which is nearly 1.00 eV lower than that on the pure Ni surface. The BaTiO₃ base not only induces wrinkling distortion of the Ni surface, which facilitates the step of CO hydrogenation, but also results in an upshift of the d-band centre and Fermi level of the catalyst, which enhances the binding strength of the catalyst with the reaction intermediates. Based on the projected density of states (PDOS) analysis, the BaTiO₃ base strongly promotes the σ-bonding interaction between the Ni surface and CO. The stronger adsorption of CO on the surface of the BaTiO₃ supported Ni catalyst results in the reduction reaction selectively generating CH₄ but not CO.

太阳能光热催化还原CO ₂是一种具有巨大潜力的化学CO ₂转化的有效方法。了解其反应机理对于开发新催化剂至关重要。在这项工作中，使用密度泛函理论 (DFT) 研究了 BaTiO _{3负载的 Ni 催化剂上 CO 2还原的机理。}BaTiO _{3碱的存在对CO 2}的吸附和活化具有重要意义。BaTiO _{3负载Ni催化剂上CO 2}还原的主要反应路径计算为CO ₂ (g)→CO ₂ →CO→COH→HCOH→CH→CH₂ →CH ₃ →CH ₄ →CH ₄ (g)，受CO还原的限速，相应的能垒为0.94 eV，比纯Ni表面的能垒低近1.00 eV。BaTiO ₃碱基不仅会引起 Ni 表面的褶皱变形，有利于 CO 加氢的步骤，而且会导致催化剂的d带中心和费米能级上移，从而增强催化剂与催化剂的结合强度。反应中间体。基于投影态密度 (PDOS) 分析，BaTiO ₃碱基强烈促进 Ni 表面与 CO 之间的 σ 键相互作用。CO 在 BaTiO 表面的吸附更强₃负载的Ni催化剂导致还原反应选择性地生成CH ₄但不生成CO。