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High-Density Frustrated Lewis Pair for High-Performance Hydrogen Evolution
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2022-11-24 , DOI: 10.1002/aenm.202203136 Wenhao Yu 1 , Yanyun Zhang 1 , Yingnan Qin 1 , Dan Zhang 1, 2 , Kang Liu 1 , G. A. Bagliuk 3 , Jianping Lai 1 , Lei Wang 1
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2022-11-24 , DOI: 10.1002/aenm.202203136 Wenhao Yu 1 , Yanyun Zhang 1 , Yingnan Qin 1 , Dan Zhang 1, 2 , Kang Liu 1 , G. A. Bagliuk 3 , Jianping Lai 1 , Lei Wang 1
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It is significant to develop catalysts with high-density and adjacent frustrated Lewis pair (FLP) sites. Herein, a method is designed to construct FLPs on an intermetallic alloy (IMA) with regulable acidity and basicity by using the Mott–Schottky effect. By dint of the high-density FLP site and suitable acidity and basicity on IMA, the fct-PtCo@NC displays excellent hydrogen evolution reaction performance. The catalyst fct-PtCo@NC, with high-density FLP sites, exhibits a fast water adsorption and decomposition rate, which is derived from the synergistic effect of FLP-acid sites and FLP-base sites significantly reducing the energy barrier between the two processes. Due to the FLP-base Pt site, fct-PtCo@NC has the best binding energy of hydrogen intermediates, the H3O+ generated during the reaction can accumulate on it and form an acid-like environment, and thus speed up the kinetics of the reaction. In comparison, the catalyst without FLP shows lower binding energy and the formation of H3O+ is not observed. This work opens a new horizon for the design of new-style heterogeneous FLP catalysts and the catalysts with high-density and adjacent FLP sites are expected to be used in a variety of multistep catalytic reactions.
中文翻译：
用于高性能析氢的高密度受挫路易斯对
开发具有高密度和相邻受抑路易斯对 (FLP) 位点的催化剂具有重要意义。在此，设计了一种方法，利用 Mott-Schottky 效应在具有可调节酸碱度的金属间合金 (IMA) 上构建 FLP。借助IMA上高密度的FLP位点和适宜的酸碱度，fct-PtCo@NC表现出优异的析氢反应性能。具有高密度 FLP 位点的催化剂 fct-PtCo@NC 表现出快速的水吸附和分解速率，这源于 FLP-酸位点和 FLP-碱位点的协同作用，显着降低了两个过程之间的能垒. 由于基于 FLP 的 Pt 位点，fct-PtCo@NC 具有最好的氢中间体结合能，H 3 O +反应过程中产生的 可以在其上积累并形成类酸环境，从而加快反应动力学。相比之下，没有 FLP 的催化剂显示出较低的结合能，并且没有观察到H 3 O +的形成。该工作为新型非均相FLP催化剂的设计开辟了新的视野，具有高密度和相邻FLP位点的催化剂有望用于多种多步催化反应。
更新日期：2022-11-24
中文翻译：
用于高性能析氢的高密度受挫路易斯对
开发具有高密度和相邻受抑路易斯对 (FLP) 位点的催化剂具有重要意义。在此，设计了一种方法，利用 Mott-Schottky 效应在具有可调节酸碱度的金属间合金 (IMA) 上构建 FLP。借助IMA上高密度的FLP位点和适宜的酸碱度，fct-PtCo@NC表现出优异的析氢反应性能。具有高密度 FLP 位点的催化剂 fct-PtCo@NC 表现出快速的水吸附和分解速率，这源于 FLP-酸位点和 FLP-碱位点的协同作用，显着降低了两个过程之间的能垒. 由于基于 FLP 的 Pt 位点，fct-PtCo@NC 具有最好的氢中间体结合能，H 3 O +反应过程中产生的 可以在其上积累并形成类酸环境，从而加快反应动力学。相比之下，没有 FLP 的催化剂显示出较低的结合能，并且没有观察到H 3 O +的形成。该工作为新型非均相FLP催化剂的设计开辟了新的视野，具有高密度和相邻FLP位点的催化剂有望用于多种多步催化反应。
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