Holey platinum nanotubes for ethanol electrochemical reforming in aqueous solution  

多孔铂纳米管用于水溶液中乙醇的电化学重整

作　　者：Tian-Jiao Wang Hui-Ying Sun Qi Xue Ming-Jun Zhong Fu-Min Li Xinlong Tian Pei Chen Shi-Bin Yin Yu Chen 王天娇;孙绘滢;薛淇;钟明君;李富民;田新龙;陈沛;尹诗斌;陈煜(Key Laboratory of Macromolecular Science of Shaanxi Province,Key Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education),Shaanxi Key Laboratory for Advanced Energy Devices,School of Materials Science and Engineering,Shaanxi Normal University,Xi'an 710062,China;State Key Laboratory of Marine Resource Utilization in South China Sea,Hainan Provincial Key Lab of Fine Chemistry,School of Chemical Engineering and Technology,Hainan University,Haikou 570228,China;MOE Key Laboratory of New Processing Technology for Non-ferrous Metals and Materials,Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials,Guangxi University,Nanning 530004,China)

机构地区：[1]Key Laboratory of Macromolecular Science of Shaanxi Province,Key Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education),Shaanxi Key Laboratory for Advanced Energy Devices,School of Materials Science and Engineering,Shaanxi Normal University,Xi'an 710062,China [2]State Key Laboratory of Marine Resource Utilization in South China Sea,Hainan Provincial Key Lab of Fine Chemistry,School of Chemical Engineering and Technology,Hainan University,Haikou 570228,China [3]MOE Key Laboratory of New Processing Technology for Non-ferrous Metals and Materials,Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials,Guangxi University,Nanning 530004,China

出　　处：《Science Bulletin》2021年第20期2079-2089,M0003,共12页科学通报（英文版）

基　　金：supported by the Natural Science Foundation of Hainan Province(2019RC007);Key Research and Development Project of Hainan Province(ZDYF2020037);the National Natural Science Foundation of China(21875133 and 51873100);Natural Science Foundation of Shaanxi Province(2020JZ-23);Fundamental Research Funds for the Central Universities(GK202101005,GK201901002,2019TS007,2021CBLZ004,and 2020CSLZ012);the Innovation Team Project for Graduate Students at Shaanxi Normal University(TD2020048Y);Open Foundation of Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials at Guangxi University(2021GXYSOF02);the 111 Project(B14041)。

摘　　要：The catalytic/electrocatalytic performance of platinum(Pt)nanostructures highly relates to their morphology.Herein,we propose a facile self-template pyrolysis strategy at high temperature to synthesize one-dimensionally holey Pt nanotubes(Pt-hNTs)using Pt^(Ⅱ)-dimethylglyoxime complex(Pt^(Ⅱ)-DMG)nanorods as the reaction precursor.The coordination capability of DMG results in the generation of Pt^(Ⅱ)-DMG nanorods,whereas the reducibility of DMG at high temperature leads to the reduction of Pt^(Ⅱ)species in Pt^(Ⅱ)-DMG nanorods.During the reaction process,the inside-out Ostwald ripening phenomenon leads to the hollow morphology of Pt-hNTs.Benefiting from the physical characteristics of hollow and holey structure,Pt-hNTs with clean surface show superior electroactivity and durability for catalyzing ethanol electrooxidation as well as hydrogen evolution reaction in alkaline media.Under optimized experimental conditions,the constructed symmetric Pt-hNTs||Pt-hNTs ethanol electrolyzer only requires an electrolysis voltage of 0.40 V to achieve the electrochemical hydrogen production,demonstrating a highly energy saving strategy relative to traditional water electrolysis.铂纳米结构的催化/电催化性能与其形貌密切相关.在此,本文提出一种简单的高温自模板法热解策略,以丁二酮肟铂络合物(Pt^(Ⅱ)-DMG)纳米棒为反应前驱体合成一维多孔Pt纳米管(Pt-hNTs).DMG的强配位能力导致Pt^(Ⅱ)-DMG纳米棒生成,而DMG的高温还原性导致了Pt^(Ⅱ)-DMG中Pt^(Ⅱ)物种的还原.在合成过程中,由内而外的奥斯特瓦尔德熟化作用使得Pt-hNTs具有中空的结构;同时,空气中的氧气能有效去除Pt-hNTs表面的碳或/和碳氧化物而形成清洁表面.得益于其中空和多孔的物理特性,表面清洁的Pt-hNTs具有高比表面积、高自稳定性和快速的传质效率,使其在碱性介质中对于催化乙醇电氧化和析氢反应表现出良好的活性和稳定性.在优化的实验条件下,构建的Pt-hNTs||Pt-hNTs乙醇电解槽仅需0.4 V的电解电压即可实现电解水制氢.本工作不仅提供了一种简单高效的中空多孔Pt纳米管的合成策略,而且表明Pt-hNTs具有优异的活性和稳定性,其可应用于其他能源/环境相关的催化体系.

关 键 词：Holey platinum nanotubes High temperature pyrolysis Ethanol electrochemical reforming Ethanol oxidation reaction Hydrogen production 

分 类 号：TB383.1[一般工业技术—材料科学与工程] O643.36[理学—物理化学]