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

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

Abstract

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

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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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)65088-7

https://www.cjcatal.com/EN/Y2026/V87/I8/100

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

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