基于阳极甘油氧化电催化的碱/酸混合电解制氢研究  

Anodic Electrocatalysis of Glycerol Oxidation for Hybrid Alkali/Acid Electrolytic Hydrogen Generation

作　　者：冯辛 刘博文 郭可鑫 范林丰 王根香 次素琴[1] 温珍海[2] Xin Feng;Bo-Wen Liu;Ke-Xin Guo;Lin-Feng Fan;Gen-Xiang Wang;Su-Qin Ci;Zhen-Hai Wen(Key Laboratory of Jiangxi Province for Persistent Pollutants Control,National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization and Resources Recycle,Nanchang Hangkong University,Nanchang,330063,Jiangxi,China;CAS Key Laboratory of Design and Assembly of Functional Nanostructures,and Fujian Key Laboratory of Nanomaterials,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou,Fujian,350002,China)

机构地区：[1]南昌航空大学,江西省持久性污染物控制与资源循环利用重点实验室,江西南昌330063 [2]中国科学院福建物质结构研究所,中科院功能纳米结构设计与组装重点实验室,福建省纳米材料重点实验室,福建福州350002

出　　处：《电化学》2023年第2期29-38,共10页Journal of Electrochemistry

基　　金：financially supported by the National Natural Science Foundation of China(22168025);the Natural Science Foundation of Jiangxi Province(20192BAB203013,20202ACB L203003);CAS-Commonwealth Scientific and Industrial Research Organization(CSIRO)Joint Research Projects(121835KYSB20200039);the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(Grant.YLU-DNL Fund 2021011)。

摘　　要：耦合可再生电能的电解水制氢是一项极具前景的绿氢技术,该技术仍受限于阳极析氧反应(OER)动力学慢、过电位高等问题的限制。在阳极端采用热力学更容易的电氧化反应代替OER,可大幅降低电耗并且在阳极端获得增值产物,是电解制氢的一种新策略。甘油作为生物柴油生产的主要副产品且产能过剩,其电催化氧化(GOR)理论电位比OER低。基于此,本研究工作报道了一种耦合酸性析氢反应(HER)与碱性GOR的混合酸/碱双电解液的制氢电解器,其以泡沫镍(NF)支撑Co_(3)O_(4)纳米片(NS)电极(Co_(3)O_(4)·NSs/NF)为阳极,商用碳载铂修饰碳布电极为阴极。在阳极端,Co_(3)O_(4)·NSs/NF对GOR电催化表现出较低的过电位和转化为甲酸盐的高选择性。在该混合酸/碱双电解液电解槽中,仅仅需要额外施加0.55 V的外加电压,即可达到10 mA·cm^(-2)的产氢电解电流密度,并可以在阳极将甘油高选择性地转化为甲酸盐,其中产氢的法拉第效率接近100%。本研究工作为电解制氢提供了一条节电、阳极增值转化的技术路线。Electrolytic hydrogen production is heavily restricted by high-energy consumption majorly due to the relatively high potential of anodic oxygen evolution reaction(OER).Development of OER-alternative reaction at the anode has been recently proposed as a promising pathway to address the associated issues.In this work,we report a hybrid acid/alkali dual-electrolyte electrolyzer by coupling acidic hydrogen evolution reaction(HER)using commercial Pt/C cathode with alkaline electrocatalytic glycerol oxidation(GOR)which is implemented by developing a nickel foam(NF)supporting Co_(3)O_(4) nanosheets anode that shows low overpotential and high selectivity toward GOR for formate production.The hybrid acid/alkali electrolyzer only requires an applied voltage of 0.55 V to achieve the electrolytic current density of 10 mA·cm^(-2) for glycerol conversion into formate at the anode and H_(2) production at the cathode with the Faraday efficiency of about 100%.The present work may open a new avenue to maximize the electron utilization efficiency and implement the energy-saving green route for H_(2) generation.

关 键 词：自支撑电极 甘油电氧化 电催化 酸/碱双电解液电解 制氢 

分 类 号：TQ116.2[化学工程—无机化工] TQ426