物理化学学报 >> 2024, Vol. 40 >> Issue (12): 2408012.doi: 10.3866/PKU.WHXB202408012

论文 上一篇    

发展二元熔盐体系用于聚七嗪亚胺薄膜光阳极的制备与水氧化性能研究

苏加鑫1, 张佳琪1, 柴姝名1, 王衍坤1, 汪思波1,2,*(), 方元行1,2,*()   

  1. 1 福州大学能源与环境光催化国家重点实验室, 福州 350116
    2 福州大学中英光催化清洁能源与先进化学品及材料国际联合实验室, 福州 350108
  • 收稿日期:2024-08-20 修回日期:2024-09-19 录用日期:2024-09-19 发布日期:2024-11-09
  • 通讯作者: Email: sibowang@fzu.edu.cn (汪思波)yxfang@fzu.edu.cn (方元行)
  • 基金资助:
    国家重点研发计划(2022YFE0114800); 国家重点研发计划(2021YFA1502100); 国家自然科学基金(22075047); 国家自然科学基金(22032002); 国家自然科学基金(U1905214); 国家自然科学基金(21961142019); 111计划(D16008)

Optimizing Poly(heptazine imide) Photoanodes Using Binary Molten Salt Synthesis for Water Oxidation Reaction

Jiaxin Su1, Jiaqi Zhang1, Shuming Chai1, Yankun Wang1, Sibo Wang1,2,*(), Yuanxing Fang1,2,*()   

  1. 1 State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou 350116, China
    2 Sino-UK International Joint Laboratory on photocatalysis for Clean Energy and Advanced Chemicals & Materials, Fuzhou University, Fuzhou 350108, China
  • Received:2024-08-20 Revised:2024-09-19 Accepted:2024-09-19 Published:2024-11-09
  • Contact: Email: sibowang@fzu.edu.cn (Sibo Wang)yxfang@fzu.edu.cn (Yuanxing Fang)
  • Supported by:
    the National Key R&D Program of China(2022YFE0114800); the National Key R&D Program of China(2021YFA1502100); National Natural Science Foundation of China(22075047); National Natural Science Foundation of China(22032002); National Natural Science Foundation of China(U1905214); National Natural Science Foundation of China(21961142019); the 111 Project (D16008)(D16008)

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摘要：

开发用于水氧化反应的聚合物薄膜光阳极引起了学术界的关注，其中碳化氮类半导体材料因其卓越的性能而尤为瞩目。本研究聚焦于一种高结晶度的氮化碳材料制备与调控，即聚七嗪亚胺薄膜光阳极，发展了二元熔盐体系用于开展聚七嗪亚胺薄膜光阳极的制备及其水氧化性能研究。优化后的电极能够在相对于可逆氢电极的1.23 V的偏置电压下，在模拟太阳光照射下，其最佳光电流密度达到了365 μA·cm−2，约为无定形PCN光阳极的18倍。双熔岩体系中，NH4SCN保证了SnS2种子层的生长，而K2CO3增强了氮化碳薄膜的结晶性。原位电化学分析表明，这种盐的组合提高了光激发电荷转移效率，并将SnS2层的厚度限制在一定范围内，使得电极电阻较小。这项研究阐明了盐在合成聚七嗪亚胺光阳极中的作用，并为设计基于高结晶碳化氮的功能性薄膜提供了研究基础。

关键词: 二元熔盐, 聚七嗪亚胺, 离子热制备法, 水氧化, 光阳极

Abstract:

Polymer-based photoanodes for the water oxidation reaction have recently garnered attention, with carbon nitride standing out due to its numerous advantages. This study focuses on synthesizing crystalline carbon nitride photoanodes, specifically poly(heptazine imide) (PHI), and explores the role of salts in their production. Using a binary molten salt system, optimal photocurrent density of 365 μA·cm−2 was achieved with a voltage bias of 1.23 V versus the reversible hydrogen electrode under AM 1.5G illumination, this performance is ca. 18 times to the pristine PCN photoanode. In this process, NH₄SCN facilitates the growth of SnS2 seeding layers, while K2CO3 enhances film crystallinity. In situ electrochemical analyses show that this salt combination improves photoexcited charge transfer efficiency and minimizes resistance in the SnS2 layer. This study clarifies the role of salts in synthesizing the PHI photoanode and provides insights for designing high-crystallinity carbon nitride-based functional films.

Key words: Binary salts, Poly-heptazine-imide, Ionothermal synthesis, Water oxidation, Photoanode