三唑环功能化聚(七嗪亚胺): 利用给体-受体构型实现高效太阳驱动过氧化氢合成

doi:10.1016/S1872-2067(26)65093-0

催化学报 ›› 2026, Vol. 87: 140-155.DOI: 10.1016/S1872-2067(26)65093-0

三唑环功能化聚(七嗪亚胺): 利用给体-受体构型实现高效太阳驱动过氧化氢合成

Sue-Faye Ng^a^,^b^,^c, Joel Jie Foo^a^,^b, Karlo Nolkemper^c^,^d^,^e, Zahra Hajiahmadi^d^,^e, Jaya Bharti^c, Nannan Hou^g, Jiankang Zheng^g, Thomas D. Kühne^d^,^e^,^f, Markus Antonietti^c, Christian Mark Pelicano^c^,^*(), Wee-Jun Ong^a^,^b^,^h^,ⁱ^,^*()

^a 厦门大学马来西亚分校能源与化工学院, 马来西亚
^b 厦门大学马来西亚分校纳米能源与催化技术卓越中心(CONNECT), 马来西亚
^c 马克斯-普朗克胶体与界面研究所胶体化学系, 波茨坦, 德国
^d 高级系统理解中心(CASUS), 哥利茨, 德国
^e 亥姆霍兹德累斯顿罗森多夫研究中心, 德累斯顿, 德国
^f 德累斯顿工业大学人工智能研究所, 计算系统科学系, 德累斯顿, 德国
^g 中国科学技术大学环境科学与工程系, 中国科学院城市污染物转化重点实验室, 安徽合肥 230026, 中国
^h 厦门大学化学与化工学院, 表界面化学全国重点实验室, 福建厦门 361005, 中国
ⁱ 厦门大学古雷石化研究院, 福建漳州 363200, 中国
^j 厦门大学深圳研究院, 广东深圳 518057, 中国
^k 高丽大学工程学院化学与生物工程系, 首尔, 韩国

收稿日期:2025-09-19 接受日期:2026-01-12 出版日期:2026-08-05 发布日期:2026-06-24
通讯作者: ^*电子信箱: christianmark.pelicano@mpikg.mpg.de (C. M. Pelicano), .
weejun.ong@xmu.edu.my (W.-J. Ong).
基金资助:
国家自然科学基金(22202168);广东基础与应用基础研究基金(2021A1515111019);中华人民共和国驻马来西亚大使馆(EENG/0045);厦门大学固体表面物理化学国家重点实验室(2023X11);厦门大学马来西亚研究生奖学金(IENG/0038);厦门大学马来西亚研究基金(ICOE/0001);厦门大学马来西亚研究基金(IENG/0090);厦门大学马来西亚研究基金(XMUMRF/2021-C8/IENG/0041);厦门大学马来西亚研究基金(XMUMRF/2025-C15/IENG/0080)

Triazole ring functionalized poly(heptazine imide): Leveraging donor- acceptor configuration toward enhanced solar-driven H₂O₂ synthesis

^a School of Energy and Chemical Engineering, Xiamen University Malaysia, Selangor Darul Ehsan 43900, Malaysia
^b Center of Excellence for NaNo Energy & Catalysis Technology (CONNECT), Xiamen University Malaysia, Selangor Darul Ehsan 43900, Malaysia
^c Department of Colloid Chemistry, Max Planck Institute of Colloids and Interfaces, Potsdam 14476, Germany
^d Center for Advanced Systems Understanding (CASUS), Untermarkt 20, 02826 Görlitz, Germany
^e Helmholtz-Zentrum Dresden-Rossendorf, Bautzner Landstrasse 400, 01328 Dresden, Germany
^f Institute of Artificial Intelligence, Chair of Computational System Sciences, Technische Universitat Dresden, 01187 Dresden, Germany
^g CAS Key Laboratory of Urban Pollutant Conversion, Department of Environmental Science and Engineering, University of Science & Technology of China, Hefei 230026, Anhui, China
^h State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China
ⁱ Gulei Innovation Institute, Xiamen University, Zhangzhou 363200, Fujian, China
^j Shenzhen Research Institute of Xiamen University, Shenzhen 518057, Guangdong, China
^k Department of Chemical and Biological Engineering, College of Engineering, Korea University, 145 Anam-ro, Seongbuk-gu, Seoul 02841, Republic of Korea

Received:2025-09-19 Accepted:2026-01-12 Online:2026-08-05 Published:2026-06-24
Supported by:
National Natural Science Foundation of China(22202168);Guangdong Basic and Applied Basic Research Foundation(2021A1515111019);Embassy of the People’s Republic of China in Malaysia(EENG/0045);State Key Laboratory of Physical Chemistry of Solid Surfaces, Xiamen University(2023X11);Xiamen University Malaysia Investigatorship(IENG/0038);Xiamen University Malaysia Research Fund(ICOE/0001);Xiamen University Malaysia Research Fund(IENG/0090);Xiamen University Malaysia Research Fund(XMUMRF/2021-C8/IENG/0041);Xiamen University Malaysia Research Fund(XMUMRF/2025-C15/IENG/0080)

摘要/Abstract

摘要：

太阳能驱动过氧化氢(H₂O₂)合成是替代传统蒽醌工艺的绿色途径, 其关键挑战在于开发高效光催化剂. 本研究采用碱金属盐(NaCl/KCl/LiCl)熔融辅助的一步煅烧法, 成功将三唑基团作为电子受体引入聚庚嗪酰亚胺(PHI)骨架, 构建了具有明确供体-受体(D-A)构型的氮化碳基催化剂. 最优催化剂(KNa)展现出高效的双功能光催化活性, H₂O₂与苯甲醛(BAD)的生成速率分别达到9.32 mmol L^-1 h^-1和8.14 mmol L^-1 h^-1. 在不使用贵金属助剂的情况下, 其在420 nm处的表观量子效率高达11.58%, 电子-空穴利用率接近理论极限(89%). 性能的提升源于其独特的D-A构型: PHI骨架作为电子供体, 末端三唑基团作为电子受体, 二者协同形成了促进电荷空间分离的内建电场, 显著抑制了光生载流子的复合, 为表面反应提供了充足的动力. 机理研究表明, KNa主要通过高效的两电子路径选择性还原氧气生成H₂O₂, 同时光生空穴、超氧自由基(O₂^●-)和单线态氧(¹O₂)等活性物种驱动苯甲醇选择性氧化. 理论计算进一步阐明, 三唑基团的引入导致PHI骨架电子密度重新分布, 增强了氧气吸附与活化能力, 从而降低了反应能垒.该催化剂在糠醛合成等其他反应中也表现出良好普适性与稳定性.

综上所述，本研究通过分子工程策略成功构建了D-A型氮化碳光催化剂, 实现了H₂O₂与高值化学品的协同高效合成. 此外, 从电子结构层面深入揭示了D-A构型促进电荷分离与表面催化的内在机制, 为设计多功能光催化系统提供了新思路.

关键词: 氮化碳, 光催化剂, 电子-空穴利用, 过氧化氢制备, 苯甲醛制备

Abstract:

Light-driven synthesis of hydrogen peroxide (H₂O₂) presents an ideal pathway for sustainability as compared to the traditional anthraquinone process. Herein, we introduce a strategic approach for functionalizing poly(heptazine imide) with triazole groups via a one-step calcination process using alkali-metal salts (NaCl/KCl/LiCl). Featuring a donor-acceptor framework that promotes singlet electron dissociation, the optimal catalyst (KNa) displayed outstanding photocatalytic performance, achieving H₂O₂ production at 9.32 mmol L^-1 h^-1 and benzaldehyde (BAD) generation at 8.14 mmol L^-1 h^-1. KNa reached an apparent quantum efficiency of 11.58% at 420 nm, in the absence of noble-metal cocatalysts. It also exhibited an electron-hole utilization close to unity (89%), indicating its efficiency in driving photoredox reactions. Mechanistic studies conducted through electrochemical measurements and scavenger tests revealed that KNa facilitated a 2-electron pathway for H₂O₂production, with photogenerated charges and radicals (electron, hole, O₂^•-, ¹O₂) participating in the reaction. A shift in electron density and enhanced O₂ adsorption observed from computational analysis reflects the donor-acceptor effect of the terminal triazole units on PHI. The versatility of KNa for other photochemical reactions was also exemplified by its simultaneous generation of H₂O₂ (1.11 mmol L^-1 h^-1) and furfuraldehyde (0.75 mmol L^-1 h^-1). As such, this research paves an in-depth understanding of synergistic dual-functional photocatalysts for photoredox reactions.

Key words: Carbon nitride, Photocatalyst, Electron-hole utilization, H₂O₂ production, Benzaldehyde production

Sue-Faye Ng, Joel Jie Foo, Karlo Nolkemper, Zahra Hajiahmadi, Jaya Bharti, Nannan Hou, Jiankang Zheng, Thomas D. Kühne, Markus Antonietti, Christian Mark Pelicano, Wee-Jun Ong. 三唑环功能化聚(七嗪亚胺): 利用给体-受体构型实现高效太阳驱动过氧化氢合成[J]. 催化学报, 2026, 87: 140-155.

Sue-Faye Ng, Joel Jie Foo, Karlo Nolkemper, Zahra Hajiahmadi, Jaya Bharti, Nannan Hou, Jiankang Zheng, Thomas D. Kühne, Markus Antonietti, Christian Mark Pelicano, Wee-Jun Ong. Triazole ring functionalized poly(heptazine imide): Leveraging donor- acceptor configuration toward enhanced solar-driven H₂O₂ synthesis[J]. Chinese Journal of Catalysis, 2026, 87: 140-155.

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图/表 16

Fig. 1. XRD patterns (a) and structure (b) of KNa (PHI with terminal triazole units). FTIR spectra from 4000-500 cm-1 (c), 1450-1250 cm-1 (d) and 800-700 cm-1 (e) for K, Li, Na, KLi-Air, KLi, and KNa photocatalysts. (Blue atom: nitrogen; grey atom: carbon; white atom: hydrogen).

Fig. 2. UV-Vis spectra (a) and corresponding Tauc plot (b) for K, Li, Na, KLi-Air, KLi, and KNa photocatalysts. Inset of (a) is a photograph of the samples, illustrating the color differences among them.

Fig. 3. Low-magnification TEM (a,b), HRTEM with FFT inset (c), and SEM images (d?f) of KNa. (g-l) HAADF and EDS elemental mapping images of KNa.

Fig. 4. C 1s, K 2p (a), and N 1s (b) high-resolution XPS spectra for KNa, KLi- and KLi-Air.

Table 1 Chemical compositions of carbon nitride samples obtained from ICP-OES.

Catalyst	Element (wt%)
Catalyst	K	Li	Na
K	15.30	—	—
Li	—	4.91	—
Na	—	—	10.2
KLi-Air	5.58	1.35	—
KLi	7.74	1.63	—
KNa	11.00	—	3.25
KNa12h	9.56	—	1.09

Fig. 5. 13C SSNMR (a), the zoomed-in yellow shaded region seen in (a,b), and 1H SSNMR (c) of KLi-Air, KLi and KNa.

Fig. 6. (a) Solar-driven simultaneous H2O2 and benzaldehyde production for different carbon nitride photocatalysts. Light source: > 420 nm, 100 mW cm-2. (b) Stability test for KNa and K catalysts (Left: H2O2 concentration; Right: BAD concentration). Action spectrum (UV-Vis spectrum: left y-axis; AQE: right y-axis) of H2O2 (c) and BAD production (d) on KNa.

Fig. 7. Literature comparison based on simultaneous photocatalytic H2O2 and BAD production (a) and AQE for H2O2 production (b) (Ultrathin CN [57], TiO2 [58], NiMIL-125-NH2 [59], Bi2MoO6 [60], Hydrophobic TiO2 [61], Ti-doped Zr-based MOF [62], OPA/Fe-Zr-MOF [63], ZnIn2S4/Ni12P5/g-C3N4 [64], g-C3N4/rGO/TiO2 [65], Au doped g-C3N4 [66]). (c) Control tests. (d) Simultaneous H2O2 and furfural (FAD) production by replacing BA with furfural alcohol.

Fig. 8. EIS (a), transient photocurrent response (yellow shaded region denotes light on) (b), LSV (c), and PL (d) spectra of carbon nitride samples.

Fig. 9. Structures of KNa PHI systems with terminal amine (a) and triazole (b) units. (Blue atom: nitrogen; grey atom: carbon; white atom: hydrogen; purple atom: potassium; ochre atom: sodium).

Table 2 Mean net atomic charges (in units of elemental charge [e]) for nitrogen and carbon atoms in heptazine, with standard deviations (σ). Further details are provided in Table S10.

Atom	KNa-PHI-amine	σ	KNa-PHI-triazole	σ
Nitrogen	-0.53	0.13	-0.51	0.11
Carbon	0.56	0.04	0.55	0.03

Fig. 10. Scavenger tests with the optimal KNa catalyst (5 mmol L-1 scavenger solution). (IPA: isopropanol; TBA: tert-butanol; pBQ: p-benzoquinone; AgNO: AgNO3; DPA: diphenylamine; TEOA: triethanolamine).

Fig. 11. RRDE voltammograms (a) and H2O2 selectivity and n (number of electrons transferred) (b) for K and KNa at 1600 rpm in 0.1 mol L-1 KOH electrolyte saturated with O2 (30 min purging). (EOC: onset potential).

Fig. 12. Charge transfer mechanism for simultaneous H2O2 and benzaldehyde production on the optimal KNa photocatalyst (CBM: conduction band minimum; VBM: valence band maximum; BA: benzyl alcohol; BAD: benzaldehyde).

Fig. 13. Adsorption of O2 onto the bridging nitrogen atoms of the model systems with terminal amine (a) and triazole (b) units, showing the differences in the adsorption behavior due to the influence of terminating groups.

Fig. 14. Gibbs free energy change for H2O2 production on KNa.

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三唑环功能化聚(七嗪亚胺): 利用给体-受体构型实现高效太阳驱动过氧化氢合成

Triazole ring functionalized poly(heptazine imide): Leveraging donor- acceptor configuration toward enhanced solar-driven H₂O₂ synthesis

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三唑环功能化聚(七嗪亚胺): 利用给体-受体构型实现高效太阳驱动过氧化氢合成

Triazole ring functionalized poly(heptazine imide): Leveraging donor- acceptor configuration toward enhanced solar-driven H2O2 synthesis

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Triazole ring functionalized poly(heptazine imide): Leveraging donor- acceptor configuration toward enhanced solar-driven H₂O₂ synthesis