Ministry of Education Key Laboratory of Pollution Processes and Environmental Criteria, Tianjin Key Laboratory of Environmental Remediation and Pollution Control, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, P. R. China.
School of Energy and Environmental Engineering, Hebei University of Technology, Tianjin 300401, P. R. China.
Proc Natl Acad Sci U S A. 2023 Feb 21;120(8):e2216584120. doi: 10.1073/pnas.2216584120. Epub 2023 Feb 14.
Nitrogen oxide (NO) pollution presents a severe threat to the environment and human health. Catalytic reduction of NO with H using single-atom catalysts poses considerable potential in the remediation of air pollution; however, the unfavorable process of H dissociation limits its practical application. Herein, we report that the in situ formation of Pt cocatalytic sites (which are stabilized by Pt-Ti bonds) over Pt/TiO significantly increases NO conversion by reducing the energy barrier of H activation. We demonstrate that two H atoms of H molecule are absorbed by adjacent Pt atoms in Pt-O and Pt-Ti, respectively, which can promote the cleave of H-H bonds. Besides, Pt sites facilitate the adsorption of NO molecules and further lower the activation barrier of the whole de-NO reaction. Extending the concept to Pt/NbO and Pd/TiO systems also sees enhanced catalytic activities, demonstrating that engineering the cocatalytic sites can be a general strategy for the design of high-efficiency catalysts that can benefit environmental sustainability.
氮氧化物（NO）污染对环境和人类健康构成严重威胁。使用单原子催化剂，用 H 催化还原 NO 在空气污染治理方面具有很大的潜力；然而，H 的不利解离过程限制了其实际应用。在此，我们报告在 Pt/TiO 上原位形成 Pt 共催化位（由 Pt-Ti 键稳定）可显著提高 NO 转化率，降低 H 活化的能垒。我们证明 H 分子的两个 H 原子分别被相邻的 Pt-O 和 Pt-Ti 中的 Pt 原子吸附，这可以促进 H-H 键的断裂。此外，Pt 位有利于 NO 分子的吸附，并进一步降低整个脱 NO 反应的活化能垒。将这一概念扩展到 Pt/NbO 和 Pd/TiO 体系也可提高催化活性，表明工程共催化位可以作为设计高效催化剂的通用策略，有利于环境可持续性。
