Cited by 122Metal-Organic Frameworks: Synthesis and ApplicationsAdvanced Photocatalysis TechniquesHydrogen Storage and Materials

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Dual Modification of Metal–Organic Frameworks for Exceptional High Piezo‐Photocatalytic Hydrogen Production

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Hu, Haijun, Li, Xiaoning, Zhang, Kailai, Yan, Ge, Kong, Weixiang, Qin, Anqi, Ma, Yali, Li, Aisen, Wang, Kai, Huang, Hongwei, Sun, Xiaodong, Ma, Tianyi·2025·Advanced Materials

DOI 10.1002/adma.202419023PMC PMC12087703

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Abstract

Metal–organic frameworks (MOFs) face significant challenges in photocatalysis due to severe carrier recombination. Here, a novel approach is presented that incorporates ─NH 2 groups and Cu ions onto MOFs with a MIL‐125 skeleton, forming NH 2‐MIL‐125 and Cu‐NH 2‐MIL‐125. This modification effectively enhances the polarity of MOFs, evidenced by significantly increased d 33 values (from 1.69 to 26.21 pm/V) and notable higher dipole moments (from 6.60 to 25.99 D). Notably, it's the first demonstration of boosting MOFs piezoelectricity via a dual modulation strategy. Moreover, the polarity can be further amplified by ultrasonic vibration based on the positive piezoelectric effect, which is justified by in situ Raman spectra, COMSOL simulations, and DFT calculations, by taking into account the applied pressure. The positive impact of introduced piezoelectric effect in facilitating charge separation and transfer of Cu‐NH 2‐MIL‐125, proved by enhanced current response. Consequently, through coupling piezocatalysis and photocatalysis, the H 2 production rate of Cu‐NH 2‐MIL‐125 can be significantly enhanced to ≈2884.2 µmol·g−1·h−1, 2.76 and 9.92 times higher than that of NH 2‐MIL‐125 and MIL‐125, respectively, ranking first in all reported MOF‐based piezo‐photocatalysts. This research demonstrates the prospective opportunity for alleviating the severe carriers recombination problem for MOFs through the implantation of piezoelectric field driving force.

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Figure 1 a) The schematic diagram of the synthesis of NH2‐MIL‐125 and Cu‐NH2‐MIL‐125. b,c) SEM images of NH2‐MIL‐125 and Cu‐NH2‐MIL‐125. The inserts are their TEM images. d) EDS elemental mapping images of Cu‐NH2‐MIL‐125. e) Fourier transformed (FT) k2‐weighted EXAFS of the Cu K‐edge of Cu‐NH2‐MIL‐125. The data is not phase‐corrected. f,g) Wavelet transformed (WT) EXAFS of Cu‐NH2‐MIL‐125 and Cu‐foil samples.CC BY-NC-ND · PubMed Central

Figure 2 a) H2 production rates of photo‐catalysis, piezo‐catalysis, and piezo‐photocatalysis for MIL‐125, NH2‐MIL‐125, and Cu‐NH2‐MIL‐125. b) The Young's modulus test for Cu‐NH2‐MIL‐125. c) H2 production rates of piezo‐photocatalysis for Cu‐NH2‐MIL‐125 under different frequences. d) H2 production rates of piezo‐photocatalysis for Cu‐NH2‐MIL‐125 under different powers. e) Piezo‐photocatalytic activity of Cu‐NH2‐MIL‐125 in different sacrificial agents. f) H2 production rates of piezo‐photocatalysis for Cu‐NH2‐MIL‐125 under different water matrices. g) Cyclic stability of H2 production rates of piezo‐photocatalysis for Cu‐NH2‐MIL‐125. h) H2 production rates of piezo‐photocatalysis for Co‐NH2‐MIL‐125, Ni‐NH2‐MIL‐125 and Cu‐NH2‐MIL‐125. i) Performance comparison of piezo‐photocatalytic H2 production rates behavior over Cu‐NH2‐MIL‐125 with state‐of‐the‐art photocatalysts and piezo‐photocatalysts in previous reports.CC BY-NC-ND · PubMed Central

Figure 3 a) Butterfly‐shaped amplitude curve of MIL‐125, NH2‐MIL‐125, and Cu‐NH2‐MIL‐125. b–d) In‐situ Raman spectra of MIL‐125, NH2‐MIL‐125, and Cu‐NH2‐MIL‐125 upon different pressure at room temperature. Arrows reveal the moving trend of the peaks.CC BY-NC-ND · PubMed Central

Figure 4 a) The simulated dipole moments of MIL‐125, NH2‐MIL‐125 and Cu‐NH2‐MIL‐125. b) The COMSOL simulated stress and potential distributions of prepared samples.CC BY-NC-ND · PubMed Central

Figure 5 a) The current response for MIL‐125, NH2‐MIL‐125, and Cu‐NH2‐MIL‐125 under light irradiation, ultrasonic vibration, or ultrasonic vibration combined with light irradiation. b) EIS for prepared samples under or in the absence of ultrasonic vibration. c) ΔGH* diagram of Cu‐NH2‐MIL‐125 in the HER reaction process with and without pressure (100 MPa). d) The cyclic voltammograms (CV) tests for NH2‐MIL‐125 and Cu‐NH2‐MIL‐125. e) The catalytic mechanism of Cu‐NH2‐MIL‐125.CC BY-NC-ND · PubMed Central

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Authors: Hu, H., Li, X., Zhang, K., Yan, G., Kong, W., Qin, A., Ma, Y., Li, A., Wang, K., Huang, H., Sun, X., & Ma, T.
Affiliations: Liaoning University (CN)
Australian Research Council (AU)
Shenyang University of Chemical Technology (CN)
Liaocheng University (CN)
China University of Geosciences (Beijing) (CN)
Corresponding author: Sun, Xiaodong
Ma, Tianyi
ORCID: Li, Xiaoning
Zhang, Kailai
Yan, Ge
Ma, Yali
Li, Aisen
Wang, Kai
Huang, Hongwei
Sun, Xiaodong
Ma, Tianyi
Venue: Advanced Materials
Publisher: Wiley
Published: 2025-03-30
Volume: 37
Issue: 20
Pages: e2419023-e2419023
ISSN: 0935-9648 (ISSN-L)
1521-4095
DOI: 10.1002/adma.202419023
PMC: PMC12087703
OpenAlex: W4409023411
Cited by: 122
References: 42
Citations by year: 2026: 85 · 2025: 37
FWCI: 26.67
Type: journal article
Language: en
Open access: hybrid
doi.org
Licence: cc-by-nc-nd
creativecommons.org/licenses/by-nc-nd/4.0/ (vor)
Locations: Advanced Materials (publishedVersion, cc-by-nc-nd)
PubMed Central (publishedVersion, cc-by-nc-nd)
PubMed (publishedVersion)
Funders: National Natural Science Foundation of China (22101105, 52071171, 52202248, 22401198)
Topics: Physical Sciences › Chemistry › Inorganic Chemistry › Metal-Organic Frameworks: Synthesis and Applications
Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Advanced Photocatalysis Techniques
Physical Sciences › Materials Science › Materials Chemistry › Hydrogen Storage and Materials
Keywords: metal-organic frameworks, piezo-photocatalysis, hydrogen production, MIL-125(Ti), amine functionalization, copper doping, piezoelectric properties, charge recombination, charge separation, ultrasonic vibration, piezoelectric field, dipole moment, piezoelectric coefficient

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Dual Modification of Metal–Organic Frameworks for Exceptional High Piezo‐Photocatalytic Hydrogen Production

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