Decoupling hydrogen production from water oxidation by integrating a triphase interfacial bioelectrochemical cascade reaction  

基于三相界面生物电化学级联反应的高效制氢研究

作　　者：Jun Zhang Xia Sheng Zhenyao Ding Haili Wang Lai Feng Xiqi Zhang Liping Wen Lei Jiang Xinjian Feng 张军;盛夏;丁臻尧;王海丽;冯莱;张锡奇;闻利平;江雷;封心建(College of Chemistry,Chemical Engineering and Materials Science,Soochow University,Suzhou 215123,China;College of Energy,Soochow Institute for Energy and Materials Innovations,Soochow University,Suzhou 215006,China;Key Laboratory of Bio-inspired Materials and Interfacial Science,Technical Institute of Physics and Chemistry,Chinese Academy of Sciences,Beijing 100190,China;School of Future Technology,University of Chinese Academy of Sciences,Beijing 101407,China)

机构地区：[1]College of Chemistry,Chemical Engineering and Materials Science,Soochow University,Suzhou 215123,China [2]College of Energy,Soochow Institute for Energy and Materials Innovations,Soochow University,Suzhou 215006,China [3]Key Laboratory of Bio-inspired Materials and Interfacial Science,Technical Institute of Physics and Chemistry,Chinese Academy of Sciences,Beijing 100190,China [4]School of Future Technology,University of Chinese Academy of Sciences,Beijing 101407,China

出　　处：《Science Bulletin》2021年第2期164-169,M0004,共7页科学通报（英文版）

基　　金：supported by the National Key R&D Program of China(2019YFA0709200);the National Natural Science Foundation of China(21988102,51772198 and 21975171)。

摘　　要：Water electrolysis to produce H2 is a promising strategy for generating a renewable fuel.However,the sluggish-kinetics and low value-added anodic oxygen evolution reaction(OER)restricts the overall energy conversion efficiency.Herein we report a strategy of boosting H_(2)production at low voltages by replacing OER with a bioelectrochemical cascade reaction at a triphase bioanode.In the presence of oxygen,oxidase enzymes can convert biomass into valuable products,and concurrently generate H_(2)O_(2) that can be further electrooxidized at the bioanode.Benefiting from the efficient oxidase kinetics at an oxygen-rich triphase bioanode and the more favorable thermodynamics of H_(2)O_(2)oxidation than that of OER,the cell voltage and energy consumption are reduced by~0.70 V and~36%,respectively,relative to regular water electrolysis.This leads to an efficient H_(2)production at the cathode and valuable product generation at the bioanode.Integration of a bioelectrochemical cascade into the water splitting process provides an energy-efficient and promising pathway for achieving a renewable fuel.电解水是一种极具前景的制氢方法.但是,由于阳极析氧反应(OER)存在过电位高、反应动力学迟缓及产物氧气附加值低等问题,限制了其能量转换效率和广泛应用.本文报道了一种利用三相界面生物电化学级联反应来代替OER,提高电解水制氢效率的方法.在氧气的存在下,氧化酶可以将生物质转化为高附加值的产物,同时生成具有高电还原活性的H_(2)O_(2).得益于高效的三相界面氧化酶催化反应动力学以及低的H_(2)O_(2)电化学氧化电位,与常规电解水相比,基于三相界面生物阳极电解制氢的电压和能耗分别降低了~0.70 V和~36%.并且,在实现高效制氢的同时,还获得了高附加值的酶催化反应产物.将生物电化学级联反应与电化学还原水制氢进行耦合,为可再生燃料的制备提供了一种有效途径.

关 键 词：Hydrogen production Water electrolysis OXIDASE Bioelectrochemical cascade reaction 

分 类 号：TQ116.2[化学工程—无机化工]