Wu Xiaomin, Sun Shaodi, Wang Ruichen, Huang Zhiwei, Shen Huazheng, Zhao Huawang, Jing Guohua
Department of Environmental Science & Engineering, College of Chemical Engineering, Huaqiao University, Xiamen, Fujian 361021, PR China.
Department of Environmental Science & Engineering, College of Chemical Engineering, Huaqiao University, Xiamen, Fujian 361021, PR China.
J Hazard Mater. 2023 Jul 15;454:131434. doi: 10.1016/j.jhazmat.2023.131434. Epub 2023 Apr 27.
Achieving high atomic utilization and low cost of desirable Pt/TiO catalysts is a major challenge for room temperature HCHO oxidation. Here, the strategy of anchoring stable Pt single atoms by abundant oxygen vacancies over TiO-nanosheet-assembled hierarchical spheres (Pt/TiO-HS) was designed to eliminate HCHO. A superior HCHO oxidation activity and CO yield (∼100% CO yield) at relative humidity (RH) > 50% over Pt/TiO-HS is achieved for long-term run. We attribute the excellent HCHO oxidation performance to the stable isolated Pt single atoms anchored on the defective TiO-HS surface. The Pt on the Pt/TiO-HS surface has a facile intense electron transfer with the support by forming Pt-O-Ti linkages, driving HCHO oxidation effectively. Further in situ HCHO-DRIFTS revealed that the dioxymethylene (DOM) and HCOOH/HCOO intermediates were further degraded via active OH and adsorbed oxygen on the Pt/TiO-HS surface, respectively. This work may pave the way for the next generation of advanced catalytic materials for high-efficiency catalytic HCHO oxidation at room temperature.
实现具有高原子利用率和低成本的理想Pt/TiO催化剂是室温下甲醛氧化面临的一项重大挑战。在此，设计了通过TiO纳米片组装的分级球体（Pt/TiO-HS）上丰富的氧空位来锚定稳定的Pt单原子的策略，以消除甲醛。在相对湿度（RH）>50%的条件下，Pt/TiO-HS在长期运行中实现了优异的甲醛氧化活性和CO产率（~100%的CO产率）。我们将优异的甲醛氧化性能归因于锚定在有缺陷的TiO-HS表面的稳定孤立Pt单原子。Pt/TiO-HS表面的Pt通过形成Pt-O-Ti键与载体进行 facile 强烈的电子转移，有效地驱动甲醛氧化。进一步的原位甲醛漫反射红外傅里叶变换光谱（HCHO-DRIFTS）表明，二氧亚甲基（DOM）和HCOOH/HCOO中间体分别通过Pt/TiO-HS表面的活性OH和吸附氧进一步降解。这项工作可能为下一代用于室温下高效催化甲醛氧化的先进催化材料铺平道路。
