内建电场耦合非贵金属等离基元效应助推MIL-125光催化二氧化碳还原活性

doi:10.1016/S1872-2067(26)65088-7

催化学报 ›› 2026, Vol. 87: 100-112.DOI: 10.1016/S1872-2067(26)65088-7

内建电场耦合非贵金属等离基元效应助推MIL-125光催化二氧化碳还原活性

姜晓康^a^,¹, 高永泽^a^,¹, 张博闻^a^,¹, 杨晓东^a, 袁之敏^b^,^*(), 许兆宁^a, 孙彬^c^,^*(), 姜在勇^b, 周国伟^c^,^*(), 周恩龙^a^,^*()

^a 山东农业大学化学与材料科学学院, 山东泰安 271018
^b 潍坊学院化学化工与环境工程学院, 山东潍坊 261061
^c 齐鲁工业大学(山东省科学院)化学与化工学院, 山东济南 250353

收稿日期:2025-12-01 接受日期:2026-01-12 出版日期:2026-08-18 发布日期:2026-06-24
通讯作者: ^*电子信箱: yuanzhiminjinan@163.com (袁之敏),
binsun@qlu.edu.cn (孙彬),
gwzhou@qlu.edu.cn (周国伟),
chemelzhou@sdau.edu.cn (周恩龙).
作者简介:¹共同第一作者.
基金资助:
国家自然科学基金(22502145);国家自然科学基金(22572148);国家自然科学基金(52202102);国家自然科学基金(52472215);国家自然科学基金(61804075);山东省自然科学基金(ZR2023MB049);山东省自然科学基金(ZR2023QB285)

Built-in electric field coupled with non-noble metal plasma cocatalyst boosts photocatalytic CO₂ reduction of MIL-125

Xiaokang Jiang^a^,¹, Yongze Gao^a^,¹, Bowen Zhang^a^,¹, Xiaodong Yang^a, Zhimin Yuan^b^,^*(), Zhaoning Xu^a, Bin Sun^c^,^*(), Zaiyong Jiang^b, Guowei Zhou^c^,^*(), Enlong Zhou^a^,^*()

^a College of Chemistry and Material Science, Shandong Agricultural University, Taian 271018, Shandong, China
^b School of Chemistry & Chemical Engineering and Environmental Engineering, Weifang University, Weifang 261061, Shandong, China
^c School of Chemistry and Chemical Engineering, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250353, Shandong, China

Received:2025-12-01 Accepted:2026-01-12 Online:2026-08-18 Published:2026-06-24
About author:¹Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(22502145);National Natural Science Foundation of China(22572148);National Natural Science Foundation of China(52202102);National Natural Science Foundation of China(52472215);National Natural Science Foundation of China(61804075);Natural Science Foundation of Shandong Province, China(ZR2023MB049);Natural Science Foundation of Shandong Province, China(ZR2023QB285)

摘要/Abstract

摘要：

利用太阳能驱动半导体光催化还原CO₂是实现碳循环与可再生能源转化的重要途径. 金属有机框架(MOF)材料因其高比表面积和优异的CO₂吸附能力而备受关注, 但光吸收范围窄、光生载流子分离效率低等问题限制了其光催化性能. 等离子体助催化剂修饰被认为是提升无机半导体材料光吸收能力和载流子分离效率的有效策略, 现也开始在MOF基光催化剂中被探索和应用. 由于金属与MOF之间存在固有晶格失配与生长条件差异, 导致它们之间存在较大的界面势垒, 阻碍光电子有效传输, 限制了其光催化应用. 构筑内建电场可作为驱动力克服界面势垒, 促进电荷分离与迁移的有效策略, 而这在金属/MOF光催化领域鲜有报道. 基于此, 如果在非贵金属等离子体金属/MOF复合材料界面构筑内建电场, 将有效地拓宽MOF的光吸收范围、促进光生载流子分离, 为突破MOF基材料光催化性能瓶颈、提升光催化还原CO₂活性提供关键解决方案.

本文采用溶剂热法, 以Bi(NO₃)₃·5H₂O为铋源, 在MIL-125表面原位还原沉积Bi纳米颗粒, 制备了一系列具有内建电场和等离激元效应的BM-X复合光催化剂. 在模拟太阳光照射, 无外加牺牲试剂条件下, 最优的BM-110光催化还原CO₂的CO产率达96.63 μmol g^‒1 h^‒1, 为原始MIL-125的10.4倍, 选择性高达97%. X-射线粉末衍射、扫描电镜、透射电镜、电子顺磁共振光谱、比表面积等结果证实Bi纳米颗粒成功负载于MIL-125表面, 并发现Bi³⁺的蚀刻作用可在MIL-125中引入氧空位和介孔结构, 有利于增强CO₂和H₂O的传质. 紫外-可见吸收光谱、莫特-肖特基测试、电化学阻抗谱、荧光光谱等光电化学测试表明, BM-110具有更宽的光吸收范围、更高的载流子浓度与更有效的电荷分离效率. 密度泛函理论计算与原位X-射线光电子能谱揭示了Bi与MIL-125之间形成由Bi指向MIL-125的内置电场, 促进光生电子从MIL-125向Bi转移, 同时Bi表面发生动态Bi³⁺/Bi⁰氧化还原循环, 进一步增强等离子体效应与光催化活性.

综上, 该体系光催化还原CO₂性能的显著提升可归因于Bi的等离子体效应拓宽光吸收、内建电场驱动界面电子迁移、氧空位促进载流子捕获与反应物活化等多重机制的协同作用赋予了Bi/MIL-125光催化剂优异的光吸收能力、高效的光生载流子空间分离与转移效率. 本研究通过非贵金属等离基元效应与内建电场的协同设计, 为构建高效MOF基光催化还原二氧化碳催化剂提供了新思路, 对高效人工光合作用系统的开发具有重要借鉴价值.

关键词: 金属铋, MIL-125, 等离子体效应, 内建电场, 光催化还原CO₂

Abstract:

In recent years, metal-organic frameworks (MOFs) based materials have garnered significant interest for photocatalytic CO₂ reduction, owing to their unique structural features coupled with exceptional CO₂ capture capacities. Due to the insufficient light absorption capacity and low efficiency of photogenerated electron-hole separation, their catalytic activities still need to be further improved. Plasma cocatalyst is considered as a promising strategy to expand light absorption range and facilitate separation efficiency of photogenerated charges for inorganic semiconductor photocatalysts, thereby also beginning to be explored and applied in the MOFs-based photocatalysts. However, due to the usual lattice mismatch or large growth differences between metals and MOFs, interface barriers exist, which to some extent hinders the effective transmission of photogenerated electrons. Build-in electric field (IEF) of the interface could be used as the driving force to overcome the interface barriers, promoting the transfer of charge carriers. Herein, the non-noble metal Bi and ordinary MIL-125 are chosen as plasma cocatalyst and MOF object, respectively, forming Bi/MIL-125 composite via an in-situ reduction strategy. The experimental results and theoretical calculation demonstrate that an IEF is formed and pointed from Bi to MIL-125. And metal Bi possesses obvious plasma light absorption and carrier capture capabilities. Built-in electric field in coordination with Bi plasma co-catalytic effect realizes the highly efficient photocatalytic CO₂ reduction. The optimized BM-110 demonstrates a 10.4-fold higher CO production rate relative to the initial MIL-125, recording a yield of 96.63 µmol g^‒1 h^‒1. This work demonstrated a new insight to design MOF-based photocatalysts for photocatalytic CO₂ reduction.

Key words: Metal Bi, MIL-125, Plasma effect, Built-in electric field, Photocatalytic CO₂ reduction

姜晓康, 高永泽, 张博闻, 杨晓东, 袁之敏, 许兆宁, 孙彬, 姜在勇, 周国伟, 周恩龙. 内建电场耦合非贵金属等离基元效应助推MIL-125光催化二氧化碳还原活性[J]. 催化学报, 2026, 87: 100-112.

Xiaokang Jiang, Yongze Gao, Bowen Zhang, Xiaodong Yang, Zhimin Yuan, Zhaoning Xu, Bin Sun, Zaiyong Jiang, Guowei Zhou, Enlong Zhou. Built-in electric field coupled with non-noble metal plasma cocatalyst boosts photocatalytic CO₂ reduction of MIL-125[J]. Chinese Journal of Catalysis, 2026, 87: 100-112.

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图/表 8

Fig. 1. (a) The prepared scheme of BM catalyst. XRD patterns (b) and FT-IR spectra (c) of MIL-125 and BM-X. (d) The nitrogen adsorption-desorption isotherms of BM-110 and MIL-125. (e) Pore size distribution of BM-110 and MIL-125.

Fig. 2. SEM images of MIL-125 (a) and BM-110 (b,c). TEM images of MIL-125 (d) and BM-110 (e,f). (g,h) HR-TEM images of BM-110. (i) Elemental mappings of Ti, C, O and Bi for BM-110.

Fig. 3. XPS spectra of MIL-125 and BM-110: survey spectra (a), Ti 2p (b), and O 1s (c). (d) EPR spectra of MIL-125 and BM-110. (e) In-situ XPS spectra of Bi 4f. (f) Charge transfer path of the BM-110 under light. (g) The formation rate of reduction products. (h) The electron selectivity of CO and CH4. (i) CO evolution yield via using as-prepared photocatalysts.

Fig. 4. Photocatalytic stability test of BM-110 (a) and photocatalytic CO2 reduction performance under different test conditions by BM-110 (b). UV-vis DRS (c), Tauc plots (d), Mott-Schottky plot (e), EIS Nyquist plots (f), transient photocurrent (g), PL spectra (h), and TRPL decay curves (i) of MIL-125 and BM-110.

Table 1 TRPL double-exponential decay time constants for MIL-125 and BM-110.

Simple	τ₁ (ns)	A₁ (Rel%)	τ₂ (ns)	A₂ (Rel%)	τ_ave (ns)
MIL-125	0.91	43.3	5.06	56.7	4.56
BM-110	1.25	46.93	6.15	53.07	5.40

Fig. 5. Plots for DFT calculated differential charge density for heterojunction formation between the MIL-125 and the Bi layers (a?c) and planar-averaged differential charge density (d) of BM-110. (The electrons accumulation and depletion are represented by the yellow and blue regions, respectively; the charge transfer was quantified by Bader charge analyses). DOS of MIL-125 (e) and Bi/MIL-125 (f). Work functions of MIL-125 (g), Bi (h) and BM-110 (i). See the Supporting Information for computational details.

Fig. 6. (a) Schematic of the setup used for KPFM measurements. AFM (b) and KPFM (c) images of BM-110 in darkness. (d) KPFM image of BM-110 in illumination. (e) Surface potential difference in darkness and light.

Fig. 7. (a) In-situ DRIFTS spectra for photocatalytic reduction of CO2 on BM-110. (b) Photocatalytic reaction mechanism of BM-110.

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内建电场耦合非贵金属等离基元效应助推MIL-125光催化二氧化碳还原活性

Built-in electric field coupled with non-noble metal plasma cocatalyst boosts photocatalytic CO₂ reduction of MIL-125

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内建电场耦合非贵金属等离基元效应助推MIL-125光催化二氧化碳还原活性

Built-in electric field coupled with non-noble metal plasma cocatalyst boosts photocatalytic CO2 reduction of MIL-125

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Built-in electric field coupled with non-noble metal plasma cocatalyst boosts photocatalytic CO₂ reduction of MIL-125