具有光诱导双缺陷的WO3/PHI S型异质结用于高选择性光催化CO2转化为CO

doi:10.1016/S1872-2067(26)65232-1

催化学报 ›› 2027, Vol. 92: 219-236.DOI: 10.1016/S1872-2067(26)65232-1

具有光诱导双缺陷的WO₃/PHI S型异质结用于高选择性光催化CO₂转化为CO

刘梦萱^a, 张荣鑫^b, 张欣^b^,^*(), 张艳峰^a^,^*()

^a 河北师范大学化学与材料科学学院, 无机纳米材料河北重点实验室, 河北石家庄 050024
^b 湖北文理学院功能材料研究院, 低维光电材料与器件湖北省重点实验室, 湖北襄阳 441053

收稿日期:2026-06-22 接受日期:2026-08-11 出版日期:2027-01-02 发布日期:2026-10-30
通讯作者: *电子信箱: zhangyanfeng@hebtu.edu.cn (张艳峰),
xinzhang@hbuas.edu.cn (张欣).
基金资助:
河北省自然科学基金(B2022205008);河北省科技创新能力提升计划(22567604H);湖北省自然科学基金创新发展联合基金(JCZRLH202600137)

WO₃/PHI S-scheme heterojunction with photoinduced dual defects for highly selective photocatalytic CO₂-to-CO conversion

Mengxuan Liu^a, Rongxin Zhang^b, Xin Zhang^b^,^*(), Yanfeng Zhang^a^,^*()

^a National Demonstration Center for Experimental Chemistry Education, Hebei Key Laboratory of Inorganic Nano-materials, College of Chemistry and Materials Science, Hebei Normal University, Shijiazhuang 050024, Hebei, China
^b Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices, Hubei University of Arts and Science, Xiangyang 441053, Hubei, China

Received:2026-06-22 Accepted:2026-08-11 Online:2027-01-02 Published:2026-10-30
Contact: *E-mail: zhangyanfeng@hebtu.edu.cn (Y. Zhang),
xinzhang@hbuas.edu.cn (X. Zhang).
Supported by:
Hebei Provincial Natural Science Foundation(B2022205008);Innovation Capability Improvement Plan Project of Hebei Province(22567604H);Joint Foundation for Innovation and Development of Hubei Natural Science Foundation(JCZRLH202600137)

摘要/Abstract

摘要：

随着工业化进程加速和全球能源需求持续增长, 化石燃料大量燃烧导致大气CO₂浓度持续攀升, 引发温室效应加剧、极端气候频发及海洋酸化等严峻环境问题. 在“双碳”目标驱动下, 将CO₂作为碳资源进行高效转化利用, 已成为能源、环境与材料科学交叉领域的研究热点. 光催化CO₂还原技术可将太阳能直接转化为化学能, 是缓解能源危机和实现人工碳循环的理想途径之一. 然而, 单一光催化剂普遍存在光生载流子复合率高、CO₂吸附活化能力弱及产物选择性差等瓶颈, 严重制约了其实际应用. 因此, 合理设计兼具高效电荷分离、强氧化还原能力和丰富活性位点的异质结催化体系, 对提升光催化CO₂还原性能具有重要意义.

本工作通过还原剂诱导策略构建了富含氧空位(OVs)和氮空位(NVs)的WO₃/PHI S型异质结光催化剂. WO₃和PHI能带结构互补且形貌匹配, 为构建S型异质结提供了理想条件. 结果表明, 在模拟太阳光下, 优化后的WO₃/PHI异质结(WP-3)CO产率达到129.2 μmol g^-1 h^-1, 选择性高达96.1%, 分别是纯WO₃和PHI的7.9倍和6.5倍, 且经过六次循环实验后活性基本保持不变, 展现出优异的稳定性. 值得注意的是, CO与CH₄的累积产率在3 h内呈线性增长, 分别达到369.8 和15.1 μmol g^-1. X-射线光电子能谱(XPS)、电子顺磁共振(EPR)及CO₂-程序升温脱附等结果证实, 原位生成及光诱导产生的OVs和NVs双缺陷显著增强了催化剂对CO₂和H₂O分子的吸附与活化能力. 高分辨透射电镜、X-射线吸收光谱及红外光谱(FTIR)表明, WO₃与PHI界面形成W-N化学键, 作为关键电荷传输通道促进界面电子转移. 飞秒瞬态吸收光谱揭示WO₃/PHI异质结中出现62.5 ps的超快衰减路径, 归属为界面构筑的载流子转移通道, 显著快于纯WO₃和PHI组分. 原位XPS和密度泛函理论(DFT)计算进一步验证, PHI功函数较低, 接触后电子自发向WO₃迁移, 形成由PHI指向WO₃的内建电场; 光照下, WO₃导带电子与PHI价带空穴在界面处复合, 保留PHI导带高能电子和WO₃价带强氧化性空穴, 遵循S-型电荷转移路径. EPR自由基捕获实验证实, WO₃/PHI同时具备更强的^•OH和^•O₂^-生成能力, 氧化还原能力显著增强. 原位漫反射FTIR光谱捕捉到*COOH, *CO及*HCOO等关键中间体, 结合DFT自由能计算, 提出CO₂ → *CO₂ → *COOH → *CO → CO的反应路径, 其中*COOH形成为决速步. 双缺陷与W-N键协同降低反应能垒, 同时适度稳定*CO中间体, 避免过度加氢生成CH₄, 从而赋予体系优异的CO选择性. ¹³CO₂同位素标记实验进一步确认了产物碳源完全来自于反应气氛中的CO₂.

综上, 本工作系统揭示了双缺陷协同S-型电荷转移路径增强光催化CO₂还原的微观机制, 为通过界面工程和缺陷调控策略设计高效、高选择性光催化剂提供了新思路, 有望推动太阳能驱动CO₂资源化利用技术的进一步发展.

关键词: S-型异质结, 氧化钨/聚庚嗪酰亚胺, 双缺陷, 协同效应, 光催化机理

Abstract:

Photocatalytic CO₂ reduction, which converts solar energy into chemical energy, represents a highly promising strategy. However, conversion efficiency is often constrained by the poor adsorption and activation of CO₂ and H₂O molecules. Here, we report an oxygen and nitrogen-vacancy-enriched WO₃/poly(heptazine imide) (PHI) S-scheme heterojunction for efficient and selective CO₂ photoreduction. The optimized WO₃/PHI heterojunction delivers a CO evolution rate of 129.2 μmol g^-1 h^-1 with 96.1% selectivity, corresponding to 7.9- and 6.5-fold enhancements over pristine WO₃ and PHI, respectively. Experiments and theoretical calculations demonstrate that the in-situ formed and photoinduced dual vacancies facilitate adsorption of CO₂ and H₂O, thereby improving the efficiency of photocatalytic CO₂ reduction. The interfacial W-N bonds serve as critical channels to accelerate interfacial charge transfer across the WO₃/PHI heterojunction. The S-scheme charge-transfer pathway, in concert with a dual-defect interfacial architecture, promotes charge transport, substantially boosting CO₂ reduction performance. This work provides mechanistic insight into defect-assisted S-scheme photocatalysis and offers a rational strategy for designing efficient photocatalysts for solar fuel production.

Key words: S-scheme heterojunction, WO₃/poly(heptazine imide), Dual defect, Synergistic effect, Photocatalytic mechanism

刘梦萱, 张荣鑫, 张欣, 张艳峰. 具有光诱导双缺陷的WO₃/PHI S型异质结用于高选择性光催化CO₂转化为CO[J]. 催化学报, 2027, 92: 219-236.

Mengxuan Liu, Rongxin Zhang, Xin Zhang, Yanfeng Zhang. WO₃/PHI S-scheme heterojunction with photoinduced dual defects for highly selective photocatalytic CO₂-to-CO conversion[J]. Chinese Journal of Catalysis, 2027, 92: 219-236.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65232-1

https://www.cjcatal.com/CN/Y2027/V92/I1/219

图/表 14

Fig. 1. (a) Schematic illustration for synthesis of WO3/PHI. SEM micrographs of WO3 (b), PHI (c), and WO3/PHI (d). (e) HRTEM image of WO3/PHI. lattice spacing of WO3 (f) and PHI (g). EDS images of C (h), N (i), W (j), and O (k) in WO3/PHI.

Fig. 2. XRD patterns (a) and FTIR spectra (b) of WO3, PHI, and WO3/PHI. Polarized Raman mapping images of WO3 (c) and WO3/PHI (d).

Fig. 3. High-resolution XPS spectra of C 1s (a), N 1s (b), W 4f (c), and O 1s (d) for WO3, PHI and WO3/PHI under dark and illuminated conditions.

Fig. 4. W L3-edge XANES (a) and corresponding k2-weight W-L3 edge FT-EXAFS (b) of W Foil, WO3 and WO3/PHI. (c) k space of EXAFS for W Foil, WO3 and WO3/PHI. W L3-edge WT-EXAFS for W Foil (d), WO3 (e), and WO3/PHI (f). All EXAFS data are k2-weighted and not phase-corrected.

Fig. 5. Pseudocolor mapping (a-c) and relevant two-dimensional ultrafast spectral signal (d-f) of fs-TA for WO3, PHI, and WO3/PHI. Corresponding kinetic decay curves within 2000 ps of WO3 (g), PHI (h), WO3/PHI (i). The decay pathways of photogenerated carriers in WO3 (j) and WO3/PHI heterojunction (k).

Fig. 6. (a) Yield of CO and CH4 with different photocatalysts. (b) Yield of CO and CH4 in catalysts prepared by different methods. (c) Yield of CO and CH4 under different experimental conditions. (d) Yield of CO and CH4 in WP-3 with different water volume. (e) Cycle experiments of WP-3 for photocatalytic CO2 RR. (d) CO2 RR experiments via WP-3 under different illumination time. (f) Performance of different catalysts for yield of CO in photocatalytic CO2 RR.

Fig. 7. (a) UV-vis DRS of pristine WO3, PHI, and WO3/PHI. (b) Bandgap plots of pristine WO3 and PHI. (c) Mott-Schottky plots of pristine WO3 and PHI. (d) VB-XPS spectra of pristine WO3 and PHI. (e) Schematic band structures of pristine WO3 and PHI.

Fig. 8. Nyquist plots (a), instantaneous photocurrent density (b), PL spectra (c) and TRPL curves (d) of pristine WO3, PHI and WO3/PHI.

Fig. 9. N2 adsorption-desorption isotherms (a) and pore-size distribution profiles (b) of WO3, PHI and WO3/PHI. (c) EPR spectra of WO3, PHI and WO3/PHI recorded under dark and illuminated conditions in air and CO2 atmospheres.

Fig. 10. Band structures of pristine WO3 (a) and PHI (b). DOS of pristine WO3 (c) and PHI (d). Work functions of pristine WO3 (e) and PHI (f).

Fig. 11. (a) Schematic illustration of the S-scheme charge-transfer pathway in WO3/PHI. EPR spectra of DMPO-trapped •OH (b) and •O2- (c) radicals for pristine WO3, PHI and WO3/PHI.

Fig. 12. In-situ FTIR spectra of photocatalytic CO2 reduction via WO3/PHI under dark (a,b), and three-dimensional colour-mapped image of photocatalytic CO2 reduction via WO3/PHI under dark (c,d).

Fig. 13. In-situ FTIR spectra of photocatalytic CO2 reduction via WO3/PHI under illumination (a,b), and three-dimensional colour-mapped image of photocatalytic CO2 reduction via WO3/PHI under illumination (c,d).

Fig. 14. Proposed mechanism of WO3/PHI for photoreduction CO2.

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具有光诱导双缺陷的WO₃/PHI S型异质结用于高选择性光催化CO₂转化为CO

WO₃/PHI S-scheme heterojunction with photoinduced dual defects for highly selective photocatalytic CO₂-to-CO conversion

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