Serrano-Jiménez J, de la Osa A R, Sánchez P, Romero A, de Lucas-Consuegra A
Department of Chemical Engineering, School of Chemical Sciences and Technologies, University of Castilla-La Mancha, Avda. Camilo José Cela 12, E-13071 Ciudad Real, Spain.
Department of Chemical Engineering, Higher Technical School of Agronomical Engineers, University of Castilla-La Mancha, Ronda de Calatrava 7, E-13071 Ciudad Real, Spain.
Energy Fuels. 2024 May 20;38(11):10038-10049. doi: 10.1021/acs.energyfuels.4c00136. eCollection 2024 Jun 6.
A systematic study on the electrochemical reforming of monosaccharides (fructose, glucose, and xylose) using Pt-based anodic electrocatalysts is here presented for the first time to completely optimize the anodic catalyst and electrolyzer operating conditions. First, the electro-oxidation of each molecule was studied using a monometallic (Pt) and two bimetallic (PtNi and PtCo) anodic electrocatalysts supported on graphene nanoplatelets (GNPs). Tests in a three-electrode cell showed superior electrochemical activity and durability of PtNi/GNPs, especially at potentials higher than 1.2 V vs RHE, with the highest electrocatalytic activity in d-xylose electro-oxidation. Then, monometallic (Pt and Ni) and bimetallic electrocatalysts with different Pt:Ni mass ratios (1:1 and 2:1) were studied for d-xylose electro-oxidation, with the 2:1 mass ratio presenting the best results. This electrocatalyst was selected as the most suitable for scale-up to an anion-exchange membrane electrolyzer, where the optimal operating potential was determined. Additionally, stable operating conditions of the electrolyzer were achieved by cyclic H production and cathodic regeneration polarization steps. This led to suitable and reproducible H production rates throughout the production cycles for renewable hydrogen production from biomass-derived streams.
本文首次对使用铂基阳极电催化剂进行单糖（果糖、葡萄糖和木糖）的电化学重整展开系统研究，以全面优化阳极催化剂和电解槽的运行条件。首先，使用负载在石墨烯纳米片（GNPs）上的单金属（Pt）和两种双金属（PtNi和PtCo）阳极电催化剂研究了每种分子的电氧化。在三电极电池中的测试表明，PtNi/GNPs具有卓越的电化学活性和耐久性，特别是在相对于可逆氢电极（RHE）高于1.2 V的电位下，在d-木糖电氧化中具有最高的电催化活性。然后，研究了具有不同Pt:Ni质量比（1:1和2:1）的单金属（Pt和Ni）和双金属电催化剂用于d-木糖电氧化，其中2:1的质量比呈现出最佳结果。这种电催化剂被选为最适合扩大规模至阴离子交换膜电解槽的催化剂，并确定了最佳运行电位。此外，通过循环制氢和阴极再生极化步骤实现了电解槽的稳定运行条件。这导致在整个生产周期中产生合适且可重复的产氢速率，用于从生物质衍生物流中生产可再生氢气。
