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化学工业与工程 2018, Vol. 35 Issue (1) :22-28    DOI: 10.13353/j.issn.1004.9533.20161082
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g-C3N4和Pt/g-C3N4在常温常压电化学合成氨中的阴极催化性能
胡红伟, 张文, 王宇新
天津大学化工学院, 化学工程联合国家重点实验室, 天津化学化工协同创新中心, 天津市膜科学与海水淡化技术 重点实验室, 天津 300350
Performance of g-C3N4 and Pt/g-C3N4 Cathode Electrocatalyst in Electrochemical Ammonia Synthesis
Hu Hongwei, Zhang Wen, Wang Yuxin
School of Chemical Engineering and Technology, State Key Laboratory of Chemical Engineering, Co-Innovation Center of Chemical Science & Engineering, Tianjin Key Laboratory of Membrane Science and Desalination Technology, Tianjin University, Tianjin 300350, China

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摘要 

电化学法合成氨是一种有希望替代传统Haber-Bosch法的新方法,而开发一种能够高效活化N2分子的催化剂成为电化学法合成氨的关键。采用一步煅烧二氰二胺的方法制备了石墨型氮化碳(g-C3N4),并将Pt纳米颗粒沉积在g-C3N4上制备了Pt/g-C3N4。采用XRD、SEM、TEM以及XPS表征和分析了所得催化剂的晶体结构,表面微观形貌和表面元素组成。分别采用H+型Nafion膜和H+/NH4+型Nafion膜作电解质,研究了Pt/g-C3N4和g-C3N4的催化性能以及Nafion膜中NH4+的作用。结果表明,Pt/g-C3N4和g-C3N4分别作阴极催化剂时均成功合成出NH3,而Pt/g-C3N4的性能优于g-C3N4。另外,膜中引入NH4+能够促进N2的电化学还原。

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胡红伟
张文
王宇新
关键词电化学合成氨   氮化碳      Nafion膜   常温常压     
Abstract

Electrochemical ammonia synthesis has been regarded as a promising alternative to the present Haber-Bosch process for ammonia production, and the development of efficient catalyst for N2 reduction is key to the electrochemical method. In this research, g-C3N4 catalyst is prepared by the thermal polycondensation process, and Pt/g-C3N4 catalyst is obtained by reducing Pt onto g-C3N4 nanosheets with ethylene glycol. The phase composition and morphology of the two kinds of catalysts are characterized by XRD, SEM, TEM and XPS. The catalytic performance of Pt/g-C3N4 and g-C3N4 in a polymer electrolyte membrane cell is studied using Nafion membranes in H+ or H+/NH4+ form, respectively. While both Pt/g-C3N4 and g-C3N4 show certain activity towards ammonia synthesis from H2 and N2 gases under ambient temperature and pressure, Pt/g-C3N4 leads to higher ammonia yield under the same conditions. The yield of ammonia appears to be higher with the H+/NH4+-form Nafion membrane, suggesting the presence of NH4+ in the membrane, facilitates the electrochemical reduction of nitrogen.

Keywordselectrochemical synthesis of ammonia;   carbon nitride;   platinum;   Nafion membrane;   ambient temperature and pressure     
Received 2016-04-28;
Corresponding Authors: 王宇新,E-mail:yxwang@tju.edu.cn。     Email: yxwang@tju.edu.cn
About author: 胡红伟(1990-),男,硕士研究生,现从事电化学方面的研究。
引用本文:   
胡红伟, 张文, 王宇新.g-C3N4和Pt/g-C3N4在常温常压电化学合成氨中的阴极催化性能[J].  化学工业与工程, 2018,35(1): 22-28
Hu Hongwei, Zhang Wen, Wang Yuxin.Performance of g-C3N4 and Pt/g-C3N4 Cathode Electrocatalyst in Electrochemical Ammonia Synthesis[J].  Chemcial Industry and Engineering, 2018,35(1): 22-28
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