原子级晶格匹配的六方相WO3/TiO2 S型异质结用于高效光电催化甘油选择性制备二羟基丙酮

doi:10.1016/S1872-2067(26)64955-8

催化学报 ›› 2026, Vol. 82: 161-173.DOI: 10.1016/S1872-2067(26)64955-8

原子级晶格匹配的六方相WO₃/TiO₂ S型异质结用于高效光电催化甘油选择性制备二羟基丙酮

张王刚^a, 谢昊辰^a, 王虹亮^a, 田入峰^b, 刘雷^b, 王剑^a^,^*(), 刘一鸣^c^,^d^,^e^,^*()

^a太原理工大学材料科学与工程学院, 山西太原 030024
^b太原理工大学化学与化工学院, 山西太原 030024
^c太原科技大学化学工程与技术学院, 山西太原 030024
^d太原理工大学环境与生态学院, 山西太原 030024
^e太原科技大学催化转化能源耦合山西省重点实验室, 山西太原 030024

收稿日期:2025-07-11 接受日期:2025-10-11 出版日期:2026-03-18 发布日期:2026-03-05
通讯作者: * 电子信箱: wangjian@tyut.edu.cn (王剑),liuyiming01@tyut.edu.cn (刘一鸣).
基金资助:
国家自然科学基金(22278290);国家自然科学基金(22578311);山西省中央引导地方科技发展资金(YDZJSX2024D030);山西省重点研发计划(2021020660301013);山西省自然科学基金(202103021224079)

Atomic-level lattice matching in hexagonal WO₃/TiO₂ S-scheme heterojunctions for high-efficiency selective photoelectrocatalytic glycerol-to-dihydroxyacetone conversion

Wanggang Zhang^a, Haochen Xie^a, Hongliang Wang^a, Rufeng Tian^b, Lei Liu^b, Jian Wang^a^,^*(), Yiming Liu^c^,^d^,^e^,^*()

^aCollege of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024 Shanxi, China
^bCollege of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
^cSchool of Chemical Engineering and technology, Taiyuan University of Science and Technology, Taiyuan 030024, Shanxi, China
^dCollege of Environmental Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
^eShanxi Key Laboratory of Catalysis and Energy Coupling, Taiyuan University of Science and Technology, Taiyuan 030024, Shanxi, China

Received:2025-07-11 Accepted:2025-10-11 Online:2026-03-18 Published:2026-03-05
Contact: * E-mail: wangjian@tyut.edu.cn (J. Wang),liuyiming01@tyut.edu.cn (Y. Liu).
Supported by:
National Natural Science Foundation of China(22278290);National Natural Science Foundation of China(22578311);Shanxi Province Central Guidance Fund for Local Science and Technology Development Project(YDZJSX2024D030);Shanxi Province Key Research and Development Program Project(2021020660301013);Shanxi Provincial Natural Science Foundation of China(202103021224079)

摘要/Abstract

摘要：

随着全球对可再生能源与高附加值化学品需求的日益增长, 光电催化技术因其绿色和可持续的特性而成为研究前沿. 作为生物柴油生产的主要副产物, 甘油高效定向转化对实现生物质资源高值化利用具有重要意义. 然而, 传统光电催化过程面临载流子复合严重与目标产物选择性低的双重挑战. 构建异质结是有效策略, 但传统的宏观结构调控策略难以从根本上解决原子级界面晶格失配引发的根本问题, 如界面缺陷多、内建电场弱及电荷传输效率低.

针对上述问题, 本研究提出“晶格匹配工程”策略, 通过精确控制退火温度, 成功在TiO₂纳米棒上构建了具有单斜相(m-WT)和六方相(h-WT)WO₃的复合光阳极. 重点研究发现, h-WO₃晶体结构使其可在TiO₂上实现近外延生长, 形成原子级连贯界面, 晶格失配率极低(h-WT为0.027%, 远低于m-WT的2.30%). 这种原子级晶格匹配特性诱导出更强的内建电场(3.71 eV), 并优化了S型电荷转移路径. 系统表征表明, h-WT异质结显著抑制了载流子复合(抑制率达90%), 延长了载流子寿命(为TiO₂的2.64倍), 并增强了对甘油分子中仲羟基的吸附亲和力(吸附能为-1.854 eV), 从而促进了甘油氧化反应优先朝向高价值的二羟基丙酮进行, 其选择性达到35%, 是m-WT体系(16%)的1.9倍. 同时, h-WT光阳极的甘油转化率高达788.6 mmol m^-2 h^-1, 较m-WT提升40%, 并保持了超过85%的总C₃产物选择性以及40 h的运行稳定性. 开尔文探针力显微镜、原位X-射线光电子能谱、电化学石英晶体微天平等结果证实了h-WT界面处存在高效的S型电荷转移机制. 进一步结合红外光谱、电子顺磁共振、同位素标记实验与密度泛函理论计算, 揭示了表面吸附的•OH自由基在选择性断裂C-H键中的主导作用, 以及仲羟基路径在热力学上的优势, 阐明了h-WT高DHA选择性的内在机理.

综上, 本文从原子尺度揭示了界面晶格匹配在同步调控异质结电荷动力学与表面反应路径中的关键作用, 为设计高效、高选择性的生物质光电催化转化系统提供了新的理论基础和材料设计策略. 未来, 通过进一步拓展晶格匹配工程至其他催化体系, 有望在可持续能源催化领域实现更精准的界面调控与性能突破.

关键词: 六方相WO₃/TiO₂, 甘油增值, 光电化学, S型异质结, 界面工程

Abstract:

This study developed a lattice-matching engineering strategy to construct atomic-level coherent interfaces in hexagonal WO₃/TiO₂ S-scheme heterojunctions to boost photoelectrocatalytic glycerol (Gly) valorization. Through precise annealing control, hexagonal WO₃/TiO₂ achieved an ultra-low lattice mismatch (m) of 0.027%, significantly lower than the 2.30% mismatch of its monoclinic counterparts, thus inducing a strong built-in electric field (3.71 eV) and optimized S-scheme charge transfer. These features resulted in 90% suppressed carrier recombination, 2.64-fold extended carrier lifetime, and enhanced secondary hydroxyl adsorption affinity (1.854 eV), collectively steering Gly oxidation toward high-value dihydroxyacetone with 35% selectivity (1.9-fold higher than that of monoclinic systems). The heterojunction also delivered a 21% Gly conversion rate (40% higher than its monoclinic counterparts), while maintaining > 85% total C3-product selectivity and stability over 40 h. This study identified the atomic-scale interface coherence as a critical factor for synchronizing charge dynamics and surface reactions in biomass upgrading.

Key words: Hexagonal WO₃/TiO₂, Glycerol valorization, Photoelectrochemical, S-scheme heterojunction, Interface engineering

张王刚, 谢昊辰, 王虹亮, 田入峰, 刘雷, 王剑, 刘一鸣. 原子级晶格匹配的六方相WO₃/TiO₂ S型异质结用于高效光电催化甘油选择性制备二羟基丙酮[J]. 催化学报, 2026, 82: 161-173.

Wanggang Zhang, Haochen Xie, Hongliang Wang, Rufeng Tian, Lei Liu, Jian Wang, Yiming Liu. Atomic-level lattice matching in hexagonal WO₃/TiO₂ S-scheme heterojunctions for high-efficiency selective photoelectrocatalytic glycerol-to-dihydroxyacetone conversion[J]. Chinese Journal of Catalysis, 2026, 82: 161-173.

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https://www.cjcatal.com/CN/Y2026/V82/I3/161

图/表 9

Fig. 1. HRTEM images of h-WT (a) and enlarged interface of Area 1 (b). The inset in (a) shows the FFT patterns of Area 1. (c) Geometric phase analysis (GPA) results of Area 1 along the ex vector direction. (d) Schematic diagrams used to calculate the m between TiO2 and h-WO3. HRTEM images of m-WT (e) and enlarged interface of Area 2 (f). The inset in (f) shows the FFT patterns of Area 2. (g) GPA results of Area 2 along the exvector direction. (h) Schematic diagrams used to calculate the m between TiO2 and m-WO3. Expanded AC-HAADF (i) and AC-BF (j) images recorded from the boxed region in Area 3. Expanded AC-HAADF (k) and AC-BF (l) images recorded from the boxed region in Area 4. (m) STEM-EDS mapping results of h-WT.

Fig. 2. Transient photocurrent density-time profiles (a), ABPE values (b), and IPCE spectra (c) of TiO2, m-WT, and h-WT at 1.23 V vs RHE in 0.1 mol L-1 Na2SO4 with 0.1 mol L-1 Gly under AM 1.5G illumination. (d) LSV curves of the TiO2, m-WT, and h-WT photoanodes. (c) Selectivity and FE of organic products over the TiO2, m-WT, and h-WT photoanodes at 1.23 V vs. RHE (measured over a 4-h period). (e) The organic products included DHA and glyceraldehyde (GLD). (f) Production rate of DHA and GLD on the TiO2, m-WT, and h-WT photoanodes at different potentials (measured over a 4-h period).

Fig. 3. Kinetic curves for the PEC GOR over h-WT (a) and m-WT (d) at 1.23 V vs. RHE. Selectivity of organic products over the h-WT (b) and m-WT (e) photoanodes at 1.23V vs. RHE (measured over a 10-h period). Stabilities of the h-WT (c) and m-WT (f) photoanodes for the PEC GOR. Error bars represent the standard deviation of the results from three parallel repeated experiments, which is within 10%; the corresponding data are the average values.

Fig. 4. (a) UV-vis DRS spectra of TiO2, m-WO3, and h-WO3. (b) Energy diagrams of h-WO3 and TiO2. (c) High-resolution Ti 2p XPS spectra of TiO2 and h-WT. (d) High-resolution W 4f XPS spectra of h-WO3 and h-WT. (e) Potential calculation for h-WT.

Fig. 5. (a,b) KPFM surface potential images of m-WT under dark and light (AM 1.5G, 100 mW cm-2) conditions, respectively. (c) Line profile (corresponding to curve 1 in panels a and b) of the surface potential across the m-WT interface under dark and light conditions. (d,e) KPFM surface potential images of h-WT under dark and light conditions, respectively. (f) Line profile (corresponding to curve 2 in panels (d) and (e)) of the surface potential across the h-WT interface under dark and light conditions. (g,h) High-resolution XPS spectra of the W 4f (g) and Ti 2p (h) regions for h-WT under dark and light conditions. (i) Schematic diagram illustrating the S-scheme charge transfer mechanism between h-WO3 and TiO2 under illumination.

Fig. 6. (a) Mott-Schottky plots measured under AM 1.5G illumination. (b) Time-resolved transient PL decay spectra up-on excitation at 280 nm. (c) EIS plots under light irradiation (inset shows the equivalent circuit of the Nyquist plots). (d) IMPS responses. (e) Plot of the potential-dependent rate constant for charge transfer. (f) Plot of the potential-dependent rate constant for charge recombination.

Fig. 7. EQCM plots (a) and FTIR spectra (b,c) for the TiO2, m-WT, and h-WT photoanodes after absorbing isopropanol and n-propanol. (d,e) DFT-calculated energies for Gly adsorption on the TiO2, m-WT, and h-WT surfaces via the primary or secondary hydroxyl group. (f,g) Adsorption energies of the GLD and DHA adsorbed on the TiO2, m-WT, and h-WT surfaces. (h) Current density-time profiles of the h-WT photoanode at 1.23 V vs. RHE in a 0.1 mol L-1 Na2SO4 electrolyte with 0.1 mol L-1 GLY, GLD, glyceric acid (GLA), or DHA under AM 1.5G illumination. (i) Proposed reaction pathway of the GOR.

Fig. 8. FTIR spectra of the dynamic isopropanol oxidation process on TiO2 (a) and h-WT (b) under AM 1.5G (100 mW cm?2) illumination for 60 min. (c) Room-temperature ESR spectra of h-WT in different electrolytes. (d) LC-MS spectra of the DHA product of the PEC GOR in an isotope-labeled electrolyte with 10% H218O. (e) Gibbs free energy profiles of the oxidation processes involving the primary and secondary hydroxyl groups on the h-WT surface.

Fig. 9. Schematic diagram illustrating the photocatalytic GOR enhancement mechanism of the interface-matched WO3-TiO2 S-heterojunction.

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原子级晶格匹配的六方相WO₃/TiO₂ S型异质结用于高效光电催化甘油选择性制备二羟基丙酮

Atomic-level lattice matching in hexagonal WO₃/TiO₂ S-scheme heterojunctions for high-efficiency selective photoelectrocatalytic glycerol-to-dihydroxyacetone conversion

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