Chong Yanan, Chen Tingyu, Li Yifei, Lin Jiajin, Huang Wei-Hsiang, Chen Chi-Liang, Jin Xiaojing, Fu Mingli, Zhao Yun, Chen Guangxu, Wei Jiake, Qiu Yongcai, Waterhouse Geoffrey I N, Ye Daiqi, Lin Zhang, Guo Lin
School of Environment and Energy, State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, South China University of Technology, Guangzhou 510000, Guangdong, China.
National Synchrotron Radiation Research Center, 101 Hsin-Ann Road, Hsinchu Science Park, Hsinchu 30076, Taiwan.
Environ Sci Technol. 2023 Apr 11;57(14):5831-5840. doi: 10.1021/acs.est.2c09795. Epub 2023 Mar 30.
Enhancing oxygen activation through defect engineering is an effective strategy for boosting catalytic oxidation performance. Herein, we demonstrate that quenching is an effective strategy for preparing defect-rich Pt/metal oxide catalysts with superior catalytic oxidation activity. As a proof of concept, quenching of α-FeO in aqueous Pt(NO) solution yielded a catalyst containing Pt single atoms and clusters over defect-rich α-FeO (Pt/FeO-Q), which possessed state-of-the-art activity for toluene oxidation. Structural and spectroscopic analyses established that the quenching process created abundant lattice defects and lattice dislocations in the α-FeO support, and stronger electronic interactions between Pt species and FeO promote the generation of higher oxidation Pt species to modulate the adsorption/desorption behavior of reactants. diffuse reflectance infrared Fourier transform spectroscopy ( DRIFTS) characterization studies and density functional theory (DFT) calculations determined that molecular oxygen and FeO lattice oxygen were both activated on the Pt/FeO-Q catalyst. Pt/CoMnO, Pt/MnO, and Pt/LaFeO catalysts synthesized by the quenching method also offered superior catalytic activity for toluene oxidation. Results encourage the wider use of quenching for the preparation of highly active oxidation catalysts.
通过缺陷工程增强氧活化是提高催化氧化性能的有效策略。在此，我们证明骤冷是制备具有优异催化氧化活性的富含缺陷的Pt/金属氧化物催化剂的有效策略。作为概念验证，在Pt(NO)水溶液中对α-FeO进行骤冷，得到了一种在富含缺陷的α-FeO（Pt/FeO-Q）上含有Pt单原子和团簇的催化剂，该催化剂对甲苯氧化具有一流的活性。结构和光谱分析表明，骤冷过程在α-FeO载体中产生了大量晶格缺陷和晶格位错，并且Pt物种与FeO之间更强的电子相互作用促进了更高氧化态Pt物种的生成，从而调节反应物的吸附/解吸行为。漫反射红外傅里叶变换光谱（DRIFTS）表征研究和密度泛函理论（DFT）计算确定，分子氧和FeO晶格氧在Pt/FeO-Q催化剂上均被活化。通过骤冷法合成的Pt/CoMnO、Pt/MnO和Pt/LaFeO催化剂对甲苯氧化也具有优异的催化活性。这些结果鼓励更广泛地使用骤冷法来制备高活性氧化催化剂。
