Wang Qiyan, Zhang Chunlei, Shi Lei, Zeng Gaofeng, Zhang Hui, Li Shenggang, Wu Ping, Zhang Yelei, Fan Yiqiu, Liu Guojuan, Jiang Zheng, Liu Zhi, Sun Yuhan
CAS Key Laboratory of Low-carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, China; School of Chemical Sciences, University of Chinese Academy of Science, Beijing 100049, China.
CAS Key Laboratory of Low-carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, China; School of Environmental and Chemical Engineering, Shanghai University, 99 Shangda Road, Shanghai 200444, China.
iScience. 2018 Nov 30;9:487-501. doi: 10.1016/j.isci.2018.11.011. Epub 2018 Nov 10.
Supported Pt catalyst has been intensively investigated for formaldehyde elimination owing to its superior reactivity at room temperature (RT). However, the high Pt content is challenging because of its high cost. Herein, we report PbO-supported Pt catalysts with only 0.1 wt % Pt, which can achieve complete conversion of formaldehyde and reliable stability at RT under demanding conditions. Both experiments and simulations demonstrate that PbO interacts strongly with the Pt species, resulting in tight Pb-O-Pt bonding at the metal/support interface and concomitant activation of the surface lattice oxygen of the support. Moreover, PbO exhibits an extremely high capacity of formaldehyde capture through methylene glycol chemisorption rather than the common hydroxyl-associated adsorption, presenting a different reaction mechanism because the active surface lattice oxygen in the vicinity of Pt species offers improved reactivity. This work provides a valuable example for the design of an efficient catalyst for formaldehyde and potentially oxidation of other carbohydrates.
负载型铂催化剂因其在室温下具有优异的反应活性而被广泛研究用于消除甲醛。然而，高铂含量因其成本高昂而具有挑战性。在此，我们报道了仅含0.1 wt%铂的PbO负载型铂催化剂，该催化剂在苛刻条件下的室温下能够实现甲醛的完全转化和可靠的稳定性。实验和模拟均表明，PbO与铂物种强烈相互作用，导致在金属/载体界面形成紧密的Pb-O-Pt键，并伴随载体表面晶格氧的活化。此外，PbO通过亚甲基二醇化学吸附而非常见的羟基相关吸附表现出极高的甲醛捕获能力，呈现出不同的反应机理，因为铂物种附近的活性表面晶格氧提供了更高的反应活性。这项工作为设计高效的甲醛催化剂以及其他碳水化合物的潜在氧化提供了一个有价值的范例。
