Sustainable co-production of H2 and lactic acid from lignocellulose photoreforming using Pt-C3N4 single-atom catalyst

doi:10.1016/S1872-2067(25)64698-5

Chinese Journal of Catalysis ›› 2025, Vol. 74: 308-318.DOI: 10.1016/S1872-2067(25)64698-5

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Sustainable co-production of H₂ and lactic acid from lignocellulose photoreforming using Pt-C₃N₄ single-atom catalyst

Eryu Wang^a^,^e^,¹, Yi-Chun Chu^b^,¹, Wenjun Zhang^a, Yanping Wei^c, Chuanling Si^a^,^d^,^*(), Regina Palkovits^e^,^f^,^g, Xin-Ping Wu^b^,^*(), Zupeng Chen^a^,^*()

^aJiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, International Innovation Center for Forest Chemicals and Materials, Nanjing Forestry University, Nanjing 210037, Jiangsu, China
^bState Key Laboratory of Green Chemical Engineering and Industrial Catalysis, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China
^cCollege of Science, Gansu Agricultural University, Lanzhou 730070, Gansu, China
^dState Key Laboratory of Biobased Fiber Materials, Tianjin Key Laboratory of Pulp and Paper, Tianjin University of Science and Technology, Tianjin 300457, China
^eInstitute for Technical and Macromolecular Chemistry, RWTH Aachen University, Worringerweg 2, 52074 Aachen, Germany
^fInstitute for a Sustainable Hydrogen Economy (INW-2), Forschungszentrum Jülich, Marie-Curie-Str. 5, 52428 Jülich, Germany
^gMax-Planck-Institute for Chemical Energy Conversion, Stiftstr. 34-36, 45470 Mülheim an der Ruhr, Germany

Received:2025-01-15 Accepted:2025-03-06 Online:2025-07-18 Published:2025-07-20
Contact: *E-mail: sichli@tust.edu.cn (C. Si), xpwu@ecust.edu.cn (X.-P. Wu), czp@njfu.edu.cn (Z. Chen).
About author:¹Contributed equally to this work.
Supported by:
National Key Research and Development Program of China(2023YFD2200505);National Natural Science Foundation of China(22202105);Natural Science Foundation of Jiangsu Higher Education Institutions of China(21KJA150003);Innovation and Entrepreneurship Team Program of Jiangsu Province(JSSCTD202345)

Abstract

Abstract:

The co-production of hydrogen and value-added biochemicals from lignocellulose utilizing solar energy has been regarded as one of the technologies most potentially able to alleviate the current energy crisis. Here, we demonstrate a cost-effective photoreforming strategy for lignocellulose valorization using a carbon nitride-supported platinum single-atom photocatalyst. An advanced H₂ evolution rate of 6.34 mmol mol_Pt^-1 h^-1 is achieved over the optimal catalyst, which is around 4.6 and 30.5 times higher compared with the nanosized Pt counterpart and pristine carbon nitride, respectively. Meanwhile, the monosaccharides are oxidized to value-added lactic acid with >99% conversion and extraordinary selectivity up to 97%. The theoretical calculations show that with Pt incorporation, the photogenerated holes are predominantly localized on the metal sites while the photogenerated electrons are concentrated on C₃N₄, thus enhancing the effective separation of charge carriers. This work provides a promising avenue for the simultaneous production of green H₂ and bio-based chemicals by biomass photorefinery.

Key words: Carbon nitride, Single-atom catalyst, Lignocellulose photorefinery, Hydrogen, Biochemical

Eryu Wang, Yi-Chun Chu, Wenjun Zhang, Yanping Wei, Chuanling Si, Regina Palkovits, Xin-Ping Wu, Zupeng Chen. Sustainable co-production of H₂ and lactic acid from lignocellulose photoreforming using Pt-C₃N₄ single-atom catalyst[J]. Chinese Journal of Catalysis, 2025, 74: 308-318.

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Figures/Tables 5

Fig. 1. (a) Schematic illustration of the synthesis of PtSA-C3N4 via a two-step calcination approach (color codes: red, platinum; purple, chlorine; green, nitrogen; orange, carbon; blue, hydrogen). (b) AC-HAADF-STEM image of PtSA-C3N4. (c) Representing HAADF-STEM image together with the corresponding EDX elemental mappings (i.e., C, N, and Pt) of PtSA-C3N4. (d) Pt 4f XPS spectra of C3N4, PtNP-C3N4, and PtSA-C3N4. Fourier transform of Pt K-edge EXAFS spectra (e), wavelet transformed EXAFS spectra (f), and Pt K-edge XANES spectra (g) of PtSA-C3N4. The spectra of Pt foil and PtO2 were shown for comparison purposes. EXAFS fitting Pt curve at R space (h) and k space (i).

Fig. 2. Effect of the amounts of PtSA-C3N4 (wGlu = 100 mg, pH = 15, wPt = 0.35 wt%) (a), glucose (wCat. = 10 mg, pH = 15, wPt = 0.35 wt%) (b), pH (wCat. = 10 mg, wGlu = 100 mg, wPt = 0.35 wt%) (c), and loading of Pt cocatalyst (d) and per Pt atomic site (wCat. = 10 mg, wGlu = 100 mg, pH = 15) (e) on photocatalytic hydrogen production rates. (f) The photocatalytic hydrogen production rates of PtSA-C3N4 over different lignocellulosic biomass substrates (100 mg) (wCat. = 10 mg, pH = 15). (g) A summary of the yield of lactic acid oxidized from monosaccharides in previous work, and more details of these reactions are available in Table S1.

Fig. 3. Time-resolved PL spectra (a), LSV curves (b), transient photocurrent response (c), and solid-state ESR spectra (d) of C3N4, PtNP-C3N4, and PtSA-C3N4. Control experiments with different additives in the photoreforming of glucose for H2 and lactic acid production (e) and DMPO ESR spin-labeling for ?OH and ?O2- applying PtSA-C3N4 (f). (g) The proposed main reaction pathway for photoreforming of monosaccharides (XYL: xylose, XYLU: xylulose, GLU: glucose, FRU: fructose, DHA: 1,3-dihydroxyacetone, HYD: 2-hydroxypropenal, PYA: pyruvic aldehyde, LAC: lactic acid).

Fig. 4. Electron-hole distributions of the first five excitations of the C3N4 (a) and PtSA-C3N4 clusters (b). H, C, N, and Pt atoms are in white, orange, green, and red, respectively. Isosurfaces (0.002 e ?-3) of electron and hole distributions are in light green and blue, respectively.

Table 1 The first five excitations of the C3N4 and PtSA-C3N4 clusters.

Cluster	Excited state	Excitation energy (eV)	Oscillator strength, f	Major contribution
C₃N₄	S₀ → S₁	3.48	0.005	HOMO → LUMO, 63%
	S₀ → S₂	3.54	0.007	HOMO−1 → LUMO, 29% HOMO−1 → LUMO+1, 27%
	S₀ → S₃	3.65	0.010	HOMO−2 → LUMO+1, 58%
	S₀ → S₄	3.85	0.003	HOMO−3 → LUMO+1, 35%
	S₀ → S₅	3.94	0.002	HOMO−4 → LUMO, 29%
Pt_SA-C₃N₄	S₀ → S₁	1.04	0.022	HOMO → LUMO, 86%
	S₀ → S₂	1.15	0.015	HOMO → LUMO+1, 82%
	S₀ → S₃	1.69	0.018	HOMO → LUMO+2, 85%
	S₀ → S₄	1.81	0.004	HOMO−1 → LUMO+1, 74%
	S₀ → S₅	1.85	0.002	HOMO−2 → LUMO+1, 86%

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Sustainable co-production of H₂ and lactic acid from lignocellulose photoreforming using Pt-C₃N₄ single-atom catalyst

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