E Bin, Bu Lingzheng, Shao Qi, Li Yujing, Huang Xiaoqing
College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, China; Department of Materials Science and Engineering, China University of Petroleum, Beijing 102249, China.
College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, China.
Sci Bull (Beijing). 2019 Jan 15;64(1):36-43. doi: 10.1016/j.scib.2018.11.020. Epub 2018 Nov 30.
The water-gas shift (WGS) reaction is an essential industrial reaction for upgrading hydrogen (H) by removing carbon monoxide (CO), while highly efficient platinum (Pt)-based catalysts for WGS with simultaneously high activity and stability are still yet to be developed due to the poisoning issue during the reaction. Herein, we report on the porous PtPb peanut nanocrystals (porous PtPb PNCs) and porous PtPb octahedron nanocrystals (porous PtPb ONCs) with controllable ratios of Pt/Pb as extremely active and stable catalysts towards WGS reaction. It exhibits the composition-dependent activity with porous PtPb PNCs-40/ZnO being the most active for WGS to H, 16.9 times higher than that of the commercial Pt/C. The porous PtPb PNCs-40/ZnO also display outstanding durability with barely activity decay and negligible structure and composition changes after ten successive reaction cycles. X-ray photoelectron spectroscopy (XPS) results reveal that the suitable binding energy of Pt 4f and the high ratio of Pt(0) to Pt(II) in porous PtPb PNCs/ZnO and porous PtPb ONCs/ZnO are crucial for the enhanced WGS activity. The CO stripping results indicate the optimized CO adsorption strength on the Pt surface ensure the excellent WGS activity and the outstanding durability. The present work demonstrates an important advance in tuning the porous metal nanomaterials as highly efficient and durable catalysts for catalysis, energy conversion and beyond.
水煤气变换（WGS）反应是通过去除一氧化碳（CO）来提纯氢气（H）的重要工业反应，然而，由于反应过程中的中毒问题，用于WGS的同时具有高活性和稳定性的高效铂（Pt）基催化剂仍有待开发。在此，我们报道了具有可控Pt/Pb比例的多孔PtPb花生形纳米晶体（多孔PtPb PNCs）和多孔PtPb八面体纳米晶体（多孔PtPb ONCs），它们是对WGS反应极具活性和稳定性的催化剂。它表现出与组成相关的活性，其中多孔PtPb PNCs-40/ZnO对WGS制H最具活性，比商业Pt/C高16.9倍。多孔PtPb PNCs-40/ZnO还表现出出色的耐久性，经过十次连续反应循环后，活性几乎没有衰减，结构和组成变化可忽略不计。X射线光电子能谱（XPS）结果表明，多孔PtPb PNCs/ZnO和多孔PtPb ONCs/ZnO中Pt 4f合适的结合能以及Pt(0)与Pt(II)的高比例对增强WGS活性至关重要。CO脱附结果表明，Pt表面优化的CO吸附强度确保了优异的WGS活性和出色的耐久性。目前的工作展示了在将多孔金属纳米材料调制成用于催化、能量转换及其他领域的高效耐用催化剂方面的重要进展。
