离子极化工程调控聚合物氮化碳框架结构实现双氧水高效人工光合成

引用本文: 谢垚, 李双军, 陈超, 樊思宇, 陶英, 张启涛. 离子极化工程调控聚合物氮化碳框架结构实现双氧水高效人工光合成[J]. 物理化学学报, 2026, 42(5): 100183. doi: 10.1016/j.actphy.2025.100183 shu

Citation: Yao Xie, Shuangjun Li, Chao Chen, Siyu Fan, Ying Tao, Qitao Zhang. Ionic polarization engineering of polymeric carbon nitride toward efficient H₂O₂ photosynthesis[J]. Acta Physico-Chimica Sinica, 2026, 42(5): 100183. doi: 10.1016/j.actphy.2025.100183 shu

离子极化工程调控聚合物氮化碳框架结构实现双氧水高效人工光合成

谢垚 ^1, ,
李双军 ^2, ,
陈超 ^1, ,
樊思宇 ^3, ,
陶英 ^{1,
,} ,
张启涛 ^{1,
,}

1.
深圳大学微纳光电子学研究院, 二维材料光电科技国际合作联合实验室, 广东深圳 518060
2.
上海大学纳米科学与技术研究中心, 上海 200444
3.
Department of Applied Chemistry, Faculty of Engineering, Kyushu Institute of Technology, Kitakyushu 804-8550, Japan

通讯作者: Email: taoying951223@163.com (陶英); qitao-zhang@szu.edu.cn (张启涛)

摘要: 熔盐极化技术利用高温熔盐中的离子相互作用，成为一种强大但尚未充分开发的结构工程策略。该技术能实现对聚合氮化碳(PCN)的精确结构调控，为提升光催化H₂O₂合成效率提供了新思路。本研究通过调控LiCl/KCl熔盐比例，成功构建了两种不同晶相结构：以七嗪单元为主的LKCN-0.95和七嗪-三嗪给受体(D-A)结结构的LKCN-0.2。结合实验与理论分析发现，富Li⁺熔盐体系促进高度有序七嗪骨架形成，而K⁺主导体系则有利于三嗪单元的引入。优化后的七嗪主导结构和七嗪-三嗪结结构分别展现出27倍和42倍的光合成H₂O₂性能提升(3.3和5.2 mmol L⁻¹ h⁻¹)，较原始PCN(0.12 mmol L⁻¹ h⁻¹)显著提高，并保持五个循环的优异稳定性。机理研究表明，结构调控可增强电荷分离效率并优化氧吸附/活化过程，从而促进选择性2e⁻氧还原反应。该工作不仅深化了对熔盐驱动结构演变的理解，更为设计高效太阳能驱动H₂O₂人工光合成催化剂提供了可规模化制备的新方法。

关键词:

English

Ionic polarization engineering of polymeric carbon nitride toward efficient H₂O₂ photosynthesis

Yao Xie ^1, ,
Shuangjun Li ^2, ,
Chao Chen ^1, ,
Siyu Fan ^3, ,
Ying Tao ^{1,
,} ,
Qitao Zhang ^{1,
,}

1.
International Collaborative Laboratory of 2D Materials for Optoelectronic Science & Technology, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen 518060, Guangdong Province, China
2.
Research Center of Nano Science and Technology, Shanghai University, Shanghai 200444, China
3.
Department of Applied Chemistry, Faculty of Engineering, Kyushu Institute of Technology, Kitakyushu 804-8550, Japan

Corresponding author: Email: taoying951223@163.com (Ying Tao); qitao-zhang@szu.edu.cn (Qitao Zhang)

Received Date: 20 August 2025
Accepted Date: 04 September 2025
Revised Date: 04 September 2025
Available Online: 15 May 2026

Abstract: Molten salt polarization, leveraging ionic interactions in high-temperature molten salts, emerges as a powerful yet underexplored strategy for structural engineering. It enables precise structural engineering of polymeric carbon nitride (PCN), offering a promising strategy to boost photocatalytic H₂O₂ synthesis. Herein, we report a controlled modulation strategy by varying LiCl/KCl ratios in molten salts to tailor the framework structures of PCN, achieving two distinct crystalline phases: heptazine-dominated (LKCN-0.95) and heptazine-triazine donor-acceptor (D-A) junction (LKCN-0.2). By integrating experimental and theoretical analyses, we revealed that Li⁺-rich molten salts promote highly ordered heptazine frameworks, while K⁺-dominated systems enable triazine incorporation. The optimized heptazine-dominated and heptazine-triazine junction exhibited 27-fold and 42-fold enhancements in H₂O₂ photosynthesis (3.3 and 5.2 mmol L⁻¹ h⁻¹) compared to pristine PCN (0.12 mmol L⁻¹ h⁻¹), alongside exceptional stability over five cycles. Mechanistic studies demonstrated that structural modulation enhances charge separation and optimizes oxygen adsorption/activation for selective 2e⁻ oxygen reduction. This work not only advances the understanding of molten salt-driven structural evolution but also provides a scalable approach for designing efficient photocatalysts toward solar-driven H₂O₂ photosynthesis.

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

离子极化工程调控聚合物氮化碳框架结构实现双氧水高效人工光合成

通讯作者: Email: taoying951223@163.com (陶英); qitao-zhang@szu.edu.cn (张启涛)

English

Ionic polarization engineering of polymeric carbon nitride toward efficient H₂O₂ photosynthesis

Corresponding author: Email: taoying951223@163.com (Ying Tao); qitao-zhang@szu.edu.cn (Qitao Zhang)

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CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

离子极化工程调控聚合物氮化碳框架结构实现双氧水高效人工光合成

通讯作者: Email: taoying951223@163.com (陶英); qitao-zhang@szu.edu.cn (张启涛)

English

Ionic polarization engineering of polymeric carbon nitride toward efficient H2O2 photosynthesis

Corresponding author: Email: taoying951223@163.com (Ying Tao); qitao-zhang@szu.edu.cn (Qitao Zhang)

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

Ionic polarization engineering of polymeric carbon nitride toward efficient H₂O₂ photosynthesis

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs