Citation: Lixing LU, Shaoxian LIU, Jian XU, Ziqi JIN, Jiongjia CHENG, Jiyang ZHAO, Fubo WANG, Haiying WANG. [FeFe]-hydrogenase-containing compound and its photocatalytic H₂-production performance[J]. Chinese Journal of Inorganic Chemistry, ;2025, 41(12): 2584-2590. doi: 10.11862/CJIC.20250200 shu

[FeFe]-hydrogenase-containing compound and its photocatalytic H₂-production performance

Lixing LU ^{1, 2} ,
Shaoxian LIU ¹ ,
Jian XU ¹ ,
Ziqi JIN ¹ ,
Jiongjia CHENG ¹ ,
Jiyang ZHAO ¹ ,
Fubo WANG ¹ ,
Haiying WANG ^{1, 3,,}

1.
School of Environmental Science, Nanjing Xiaozhuang University, Nanjing 211171, China
2.
Gaofu New Energy Co., Ltd., Wuxi, Jiangsu 214000, China
3.
State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, China

Corresponding author: Haiying WANG, wanghaiying@nju.edu.cn
Received Date: 12 June 2025
Revised Date: 11 July 2025

Figures(6)

A compound containing [FeFe]-hydrogenase, [Fe₂((SCH₂)₂R)(CO)₆] (1) (R=4-{(1H-benzo[d]imidazol-1-yl)methyl}-anilino), was prepared and thoroughly characterized by infrared spectroscopy, single-crystal X-ray diffraction, and density functional theory calculations. Its performance as a photocatalyst for hydrogen production via water splitting was evaluated under simulated sunlight. Within 3 h, the amount of H₂ produced was 386.5 μmol, achieving a catalytic efficiency of 25.26 μmol·mg^-1·h^-1 and a turnover number (TON) of 0.45.
- [FeFe]-hydrogenase,
- photocatalysis,
- water splitting,
- hydrogen production
1. [1]
  ZOU Z G, YE J H, SAYAMA K, ARAKAWA H. Direct splitting of water under visible light irradiation with an oxide semiconductor photocatalyst[J]. Nature, 2001, 414(6864): 625-627 doi: 10.1038/414625a
2. [2]
  ARMAROLI N, BALZANI V. The future of energy supply: Challenges and opportunities[J]. Angew. Chem. ‒Int. Edit., 2007, 46(1/2): 52-66
3. [3]
  GREENING C, GRINTER R. Microbial oxidation of atmospheric trace gases[J]. Nat. Rev. Microbiol., 2022, 20(9): 513-528 doi: 10.1038/s41579-022-00724-x
4. [4]
  SCHWARTZ E, FRIEDRICH B. The H₂-metabolizing prokaryotes[M]//DWORKIN M, FALKOW S, ROSENBERG E, SCHLEIFER K H, STACKEBRANDT E. The prokaryotes: Vol. 2. New York: Springer, 2006: 496-563
5. [5]
  NOCERA D G. Solar fuels and solar chemicals industry[J]. Accounts Chem. Res., 2017, 50(3): 616-619 doi: 10.1021/acs.accounts.6b00615
6. [6]
  GRAY H B. Powering the planet with solar fuel[J]. Nat. Chem., 2009, 1(1): 7-7 doi: 10.1038/nchem.141
7. [7]
  MAEDA K, TERAMURA K, LU D L, TAKATA T, SAITO N, INOUE Y, DOMEN K. Photocatalyst releasing hydrogen from water[J]. Nature, 2006, 440(7082): 295-295 doi: 10.1038/440295a
8. [8]
  WANG X C, MAEDA K, THOMAS A, TAKANABE K, XIN G, CARLSSON J M, DOMEN K, ANTONIETTI M. A metal-free polymeric photocatalyst for hydrogen production from water under visible light[J]. Nat Mater, 2009, 8(1): 76-80 doi: 10.1038/nmat2317
9. [9]
  SIDABRAS J W, STRIPP S T. A personal account on 25 years of scientific literature on [FeFe]-hydrogenase[J]. J. Biol. Inorg. Chem., 2023, 28(4): 355-378 doi: 10.1007/s00775-023-01992-5
10. [10]
  CASTNER A T, JOHNSON B A, COHEN S M, OTT S. Mimicking the electron transport chain and active site of [FeFe] hydrogenases in one metal-organic framework: Factors that influence charge transport[J]. J. Am. Chem. Soc., 2021, 143(21): 7991-7999 doi: 10.1021/jacs.1c01361
11. [11]
  KARAYILAN M, BREZINSKI W P, CLARY K E, LICHTENBERGER D L, GLASS R S, PYUN J. Catalytic metallopolymers from [2Fe-2S] clusters: Artificial metalloenzymes for hydrogen production[J]. Angew. Chem. ‒Int. Edit., 2019, 58(23): 7537-7550 doi: 10.1002/anie.201813776
12. [12]
  GAO S, LIU Y, SHAO Y D, JIANG D Y, DUAN Q. Iron carbonyl compounds with aromatic dithiolate bridges as organometallic mimics of [FeFe] hydrogenases[J]. Coord. Chem. Rev., 2020, 402: 213081 doi: 10.1016/j.ccr.2019.213081
13. [13]
  SONG L C, GU Z C, ZHANG W W, LI Q L, WANG Y X, WANG H F. Synthesis, structure, and electrocatalysis of butterfly [Fe₂SP] cluster complexes relevant to [FeFe]-hydrogenases[J]. Organometallics, 2015, 34(16): 4147-4157 doi: 10.1021/acs.organomet.5b00560
14. [14]
  PULLEN S, FEI H H, ORTHABER A, COHEN S M, OTT S. Enhanced photochemical hydrogen production by a molecular diiron catalyst incorporated into a metal-organic framework[J]. J. Am. Chem. Soc., 2013, 135(45): 16997-17003 doi: 10.1021/ja407176p
15. [15]
  VÖLLER J S. Air-stable [FeFe] hydrogenases[J]. Nat. Catal., 2018, 1(8): 564-564 doi: 10.1038/s41929-018-0137-y
16. [16]
  BOGAN L E, LESCH D A, RAUCHFUSS T B. Synthesis of heterometallic cluster compounds from Fe₃(μ₃-Te)₂(CO)₉ and comparisons with analogous sulfide clusters[J]. J. Organomet. Chem., 1983, 250(1): 429-438 doi: 10.1016/0022-328X(83)85067-0
17. [17]
  JIN G X, WANG F B, ZHAO H R, WANG X H, LI Y L, SUN Y, CHENG J Y, SHENG X H, WANG H Y, MA J P, LIU Q K. [Fe₂S₂]-hydrogenase-mimic-containing supramolecule and coordination polymers: Syntheses, H₂ evolution properties, and their structure-function relationship study[J]. Cryst. Growth Des., 2024, 24(7): 2667-2671 doi: 10.1021/acs.cgd.4c00144
18. [18]
  BENNDORF S, SCHLEUSENER A, MÜLLER R, MICHEEL M, BARUAH R, DELLITH J, UNDISZ A, NEUMANN C, TURCHANIN A, LEOPOLD K, WEIGAND W, WÄCHTLER M. Covalent functionalization of CdSe quantum dot films with molecular [FeFe] hydrogenase mimics for light-driven hydrogen evolution[J]. ACS Appl. Mater. Interfaces, 2023, 15(15): 18889-18897 doi: 10.1021/acsami.3c00184
19. [19]
  MERINERO A D, COLLADO A, CASARRUBIOS L, GÓMEZ-GALLEGO M, RAMÍREZ DE ARELLANO C, ARELLANO C, CABALLERO A, ZAPATA F, SIERRA M A. Triazole-containing [FeFe] hydrogenase mimics: Synthesis and electrocatalytic behavior[J]. Inorg. Chem., 2019, 58(23): 16267-16278 doi: 10.1021/acs.inorgchem.9b02813
20. [20]
  JIN G X, HAN C C, ZHAO H R, WU X W, LI Y L, WANG H Y, MA J P. Small-molecules-induced metal-organic-framework-based photosensitizer for greatly enhancing H₂ production efficiency[J]. ACS Mater. Lett., 2024, 6(2): 375-383 doi: 10.1021/acsmaterialslett.3c01286
21. [21]
  CHEN X H, YANG F, HAN C C, HAN L C, WANG F B, JIN G X, WANG H Y, MA J P. [Fe₂S₂-Ag_x]-hydrogenase active-site-containing coordination polymers and their photocatalytic H₂ evolution reaction properties[J]. Inorg. Chem., 2022, 61(34): 13261-13265 doi: 10.1021/acs.inorgchem.2c01818
22. [22]
  GAO L G, XU C, SU Y J, LIU A M, MA T L. Cascaded band gap design for highly efficient electron transport layer-free perovskite solar cells[J]. Chem. Commun., 2022, 58(47): 6749-6752 doi: 10.1039/D2CC01807A
23. [23]
  COSTENTIN C, DROUET S, ROBERT M, SAVÉANT J M. Turnover numbers, turnover frequencies, and overpotential in molecular catalysis of electrochemical reactions. Cyclic voltammetry and preparative-scale electrolysis[J]. J. Am. Chem. Soc., 2012, 134(27): 11235-11242 doi: 10.1021/ja303560c
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沈阳化工大学材料科学与工程学院沈阳 110142

[FeFe]-hydrogenase-containing compound and its photocatalytic H2-production performance

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通讯作者: 陈斌, bchen63@163.com

[FeFe]-hydrogenase-containing compound and its photocatalytic H₂-production performance