Proton hydrogenation reaction in neutral media: Mechanisms, challenges, and performance enhancement strategies

doi:10.1016/S1872-2067(26)65188-1

Chinese Journal of Catalysis ›› 2026, Vol. 90: 27-51.DOI: 10.1016/S1872-2067(26)65188-1

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Proton hydrogenation reaction in neutral media: Mechanisms, challenges, and performance enhancement strategies

Jiaxuan Zhou^a, Yaodong Yu^a, Jiani Han^a^,^b, Yanxue Chao^a, Jianping Lai^a^,^*(), Lei Wang^a^,^*()

^a State Key Laboratory Base of Eco-Chemical Engineering, Ministry of Education, International Science and Technology Cooperation Base of Eco-chemical Engineering and Green Manufacturing, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, China
^b Shandong Engineering Research Center for Marine Environment Corrosion and Safety Protection, College of Environment and Safety Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, China

Received:2026-01-05 Accepted:2026-03-16 Online:2026-11-05 Published:2026-09-09
About author:Jianping Lai (Qingdao University of Science and Technology) received his PhD degree in 2017 from Changchun Institute of Applied Chemistry, Chinese Academy of Sciences. From 2017 to 2019, he did postdoctoral research at Peking University. He currently leads a research team focusing on advanced electrocatalytic materials for clean energy conversion and storage. He has coauthored more than 140 peer-reviewed papers.
Lei Wang (Qingdao University of Science and Technology) has served as a member of the Editorial Board of Chin. J. Catal. since 2020 and Nano Research since 2021. Prof. Lei Wang received his B.S. degree from Qufu Normal University (China) in 2001, and Ph.D. degree from Jilin University (China) in 2006. He conducted postdoctoral research at Shandong University from 2008 to 2010 and worked as a visiting scholar at The University of Texas at San Antonio (USA) from 2012 to 2013. Since 2015, he has been a Professor at Qingdao University of Science and Technology, and currently serves as the Director of the Cultivation Base of State Key Laboratory of Eco-chemical Engineering. He is a Distinguished Young Scholar of Shandong Province (2019) and a Taishan Scholar Distinguished Expert of Shandong Province (2025). His research interests mainly focus on inorganic solid-phase synthesis, electrocatalysis, hydrogen energy, and large-scale preparation of electrocatalysts for seawater splitting. He has published more than 400 peer-reviewed SCI papers.
First author contact:Author contributions
J.L and L.W supervised the manuscript. J.L conceived the manuscript. J.Z. wrote the manuscript. Y.Y., J.H. and Y.C. contributed to the conception and direction of the manuscript, discussion of content and editing of the manuscript.
Supported by:
National Natural Science Foundation of China(52272222);Taishan Scholar Young Talent Program(tsqn201909114);Taishan Scholar Young Talent Program(tsqn201909123);University Youth Innovation Team of Shandong Province(202201010318)

Abstract

Abstract:

Proton hydrogenation reactions underpin numerous core processes in energy conversion, chemical production, and environmental remediation. While traditional acidic environments provide ample proton sources, they pose challenges such as equipment corrosion and environmental pollution. Neutral environments effectively mitigate these issues and offer broader application compatibility. However, their extremely low proton concentrations lead to challenges including slow proton supply kinetics, intensified competitive hydrogen evolution reactions, limited mass transfer of reactants, and destabilization of the interfacial microenvironment. This review systematically analyzes the reaction mechanisms and key challenges of proton hydrogenation in neutral environments. It summarizes cutting-edge strategies for performance enhancement across three dimensions: Intrinsic catalyst structure design, enhanced interfacial proton transfer, and optimization of reaction pathways and mass transport processes. Finally, it outlines future research directions including in situ mechanism studies, catalyst stability enhancement, and system energy efficiency optimization, aiming to provide theoretical guidance for constructing efficient and stable proton hydrogenation catalytic systems in neutral environments.

Key words: Neutral-environment catalysis, Proton hydrogenation reaction, Hydrogen evolution reaction suppression, Catalyst design, Reaction engineering

Jiaxuan Zhou, Yaodong Yu, Jiani Han, Yanxue Chao, Jianping Lai, Lei Wang. Proton hydrogenation reaction in neutral media: Mechanisms, challenges, and performance enhancement strategies[J]. Chinese Journal of Catalysis, 2026, 90: 27-51.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(26)65188-1

https://www.cjcatal.com/EN/Y2026/V90/I11/27

Figures/Tables 9

Fig. 1. A summary schematic diagram of the transformation of restrictive factors into constructive drivers for the performance enhancement of proton hydrogenation in neutral media and the corresponding multi-dimensional optimization strategies.

Table 1 Characteristic comparison of proton hydrogenation reactions under different media environments.

Comparison dimension	Acidic media	Neutral media	Alkaline media
Primary proton source	H₃O⁺ (high concentration)	H₂O surface dissociation (virtually the sole source)	H₂O dissociation (buffered by OH^-)
Proton concentration/M	10⁰-10^-2	~10^-7 (very low in bulk, no effective buffering)	10^-14-10^-7 (very low in bulk, regulated by buffering at interface)
Proton supply mechanism	fast Volmer step (H₃O⁺ + e^- → H + H₂O)	H₂O dissociation as the primary pathway, slow kinetics	H₂O dissociation and OH^- buffering/consumption
Mass transport characteristics	fast proton transfer, moderate gas solubility	low gas solubility, significant mass transfer limitations; local pH prone to severe fluctuation	low gas solubility, OH^- accumulation may affect interface stability
Key focus of catalyst design	fast proton transfer, moderate gas solubility	simultaneously promoting water splitting and suppressing HER, enhancing directed proton transfer, stabilizing dynamic interface	promoting water splitting, managing OH^- accumulation, stabilizing interfacial environment
Major challenges	equipment corrosion, environmental burden, complex product separation	severely insufficient proton supply, intense HER competition, mass transfer limitations, dynamic instability of interfacial microenvironment	high initial energy barrier for water splitting, need to manage interfacial alkalinity

Table 2 Correspondence between core challenges and performance optimization strategies for proton hydrogenation in neutral media.

Core challenge	Corresponding optimization strategies and primary mechanisms	Section
Limited proton supply	single-atom catalysts: Enable efficient water dissociation sites through precisely designed coordination environments, fundamentally enhancing proton generation efficiency.	3.1, 3.2
	defect engineering: Create unsaturated coordination sites (e.g., O/S vacancies) to strengthen water molecule adsorption and activation.
	interfacial functionalization: Introduce surface functional groups (e.g., -OH) to serve as proton relays, facilitating rapid interfacial proton transfer.
	biomimetic proton transport channels: Construct directed and efficient proton conduction pathways (e.g., hydrogen-bond networks) within the material for rapid bulk proton supply.
Competitive reaction (HER)	single-atom catalysts: Finely tune the electronic structure (e.g., d-band center) of active sites via coordination engineering to optimize the hydrogen adsorption free energy (ΔG_*H), steering it away from the optimal value for HER.	3.1, 3.2
	defect engineering: Alter the local charge environment via defects to construct a proton fence, spatially or energetically hindering the HER pathway.
	dual-site synergy: Spatially decouple proton generation (e.g., Fe sites) from substrate hydrogenation (e.g., Cu sites). The hydrogen spillover mechanism directs *H consumption, cutting off the feedstock supply for HER.
	interfacial functionalization: Guide proton flow via surface functional groups to prioritize arrival at hydrogenation sites, reducing the accumulation of free *H.
Reagent mass transfer limitation	GDEs strategy: Establish a gas-liquid-solid three-phase interface, allowing gaseous reactants like CO₂ and N₂ to bypass the slow dissolution-diffusion process in the liquid phase and directly reach the catalyst surface, drastically increasing local concentration.	3.3
Complexity of reaction pathways	intrinsic catalyst design (e.g., single-atom/dual-site/defect engineering): Precisely modulate the adsorption strength for different reaction intermediates, breaking scaling relationships to steer the reaction along the desired pathway.	3.1, 3.3
	intrinsic catalyst design (e.g., single-atom/dual-site/defect engineering): Precisely modulate the adsorption strength for different reaction intermediates, breaking scaling relationships to steer the reaction along the desired pathway.
	system integration strategy (e.g., Tandem catalysis): Decompose multi-step complex reactions into sequential steps performed by different catalysts or in different reactors, simplifying control at each stage and enhancing final selectivity.
Dynamic instability of the interfacial microenvironment	introduction of buffer media: Utilize the proton buffering capacity of buffer pairs to promptly neutralize generated OH⁻, suppressing drastic local pH fluctuations.	3.2, 3.3
	system integration strategy (e.g., Membrane electrode assembly): Employ ion-exchange membranes to precisely control ion transport, preventing OH^- accumulation at the cathode interface and fundamentally stabilizing the microenvironment.
	biomimetic proton transport channels: Establish efficient proton conduction networks to rapidly balance interfacial proton concentration, mitigating polarization effects caused by proton consumption.

Table 2 Correspondence between core challenges and performance optimization strategies for proton hydrogenation in neutral media.

Core challenge	Corresponding optimization strategies and primary mechanisms	Section
Limited proton supply	single-atom catalysts: Enable efficient water dissociation sites through precisely designed coordination environments, fundamentally enhancing proton generation efficiency.	3.1, 3.2
	defect engineering: Create unsaturated coordination sites (e.g., O/S vacancies) to strengthen water molecule adsorption and activation.
	interfacial functionalization: Introduce surface functional groups (e.g., -OH) to serve as proton relays, facilitating rapid interfacial proton transfer.
	biomimetic proton transport channels: Construct directed and efficient proton conduction pathways (e.g., hydrogen-bond networks) within the material for rapid bulk proton supply.
Competitive reaction (HER)	single-atom catalysts: Finely tune the electronic structure (e.g., d-band center) of active sites via coordination engineering to optimize the hydrogen adsorption free energy (ΔG_*H), steering it away from the optimal value for HER.	3.1, 3.2
	defect engineering: Alter the local charge environment via defects to construct a proton fence, spatially or energetically hindering the HER pathway.
	dual-site synergy: Spatially decouple proton generation (e.g., Fe sites) from substrate hydrogenation (e.g., Cu sites). The hydrogen spillover mechanism directs *H consumption, cutting off the feedstock supply for HER.
	interfacial functionalization: Guide proton flow via surface functional groups to prioritize arrival at hydrogenation sites, reducing the accumulation of free *H.
Reagent mass transfer limitation	GDEs strategy: Establish a gas-liquid-solid three-phase interface, allowing gaseous reactants like CO₂ and N₂ to bypass the slow dissolution-diffusion process in the liquid phase and directly reach the catalyst surface, drastically increasing local concentration.	3.3
Complexity of reaction pathways	intrinsic catalyst design (e.g., single-atom/dual-site/defect engineering): Precisely modulate the adsorption strength for different reaction intermediates, breaking scaling relationships to steer the reaction along the desired pathway.	3.1, 3.3
	intrinsic catalyst design (e.g., single-atom/dual-site/defect engineering): Precisely modulate the adsorption strength for different reaction intermediates, breaking scaling relationships to steer the reaction along the desired pathway.
	system integration strategy (e.g., Tandem catalysis): Decompose multi-step complex reactions into sequential steps performed by different catalysts or in different reactors, simplifying control at each stage and enhancing final selectivity.
Dynamic instability of the interfacial microenvironment	introduction of buffer media: Utilize the proton buffering capacity of buffer pairs to promptly neutralize generated OH⁻, suppressing drastic local pH fluctuations.	3.2, 3.3
	system integration strategy (e.g., Membrane electrode assembly): Employ ion-exchange membranes to precisely control ion transport, preventing OH^- accumulation at the cathode interface and fundamentally stabilizing the microenvironment.
	biomimetic proton transport channels: Establish efficient proton conduction networks to rapidly balance interfacial proton concentration, mitigating polarization effects caused by proton consumption.

Fig. 2. (a) FT-EXAFS spectrum fitting of Ni SAs/OMMNC and the optimized configuration for Ni in the inset (the green, blue, red and gray spheres represent Ni, N,O and C atoms). Reprinted with permission from Ref. [67]. Copyright 2022, RSC Publishing. (b) Differential charge density of NO3- adsorbed on FeSAs/g-C3N4. Reprinted with permission from Ref. [68]. Copyright 2022, Elsevier. (c) Comparison of the NH3 yield rates (mg h−1 cm−2) of Fe-N4/CNCl and Fe-N4/CN catalysts. (d) Density functional theory calculations of reaction pathways for the NO3RR on Fe-N4 sites of Fe-N4/CN, Fe-N4/CNCl-1, Fe-N4/CN-2, and Fe-N4/CN-3. Reprinted with permission from Ref. [69]. Copyright 2025, American Chemical Society. (e) CO2 conversion at 350 °C. Reaction conditions: CO2:H2 = 1:4, weight hourly space velocity = 100 L g−1 h−1. (f) In-situ diffuse reflectance infrared Fourier transform spectroscopy over 30 min of TOS at 350 °C. Non situ and in-situ XPS spectra over 30 min of TOS at 350 °C. Reprinted with permission from Ref. [70]. Copyright 2025, Elsevier.

Fig. 3. (a) Conceptual diagram of the Cu-M-N-C structure to promote NO3RR activity. (b) NH3 yield rate of ammonia yield with electrolysis time for N-C, Cu-N-C, Fe-N-C, and Cu-Fe-NC. (c) Long-term NO3RR electrolysis and corresponding FE of NH3 for Cu-Fe-N-C. (d) The NH3 FE of ammonia yield with electrolysis time for N-C, Cu-N-C, Fe-N-C, and Cu-Fe-N-C. Reprinted with permission from Ref. [72]. Copyright 2024, RSC Publishing. (e) Free energy diagram of NO2RR. (f) NH3 yield rate and corresponding FE of NH3 for Ov-Co(OH)2/Cu at different electrode potentials. Reprinted with permission from Ref. [74]. Copyright 2025, John Wiley and Sons.

Fig. 4. (a) Possible migration routes of hydrogen spillover process for Cu1/SiO2 with surface hydroxyls. The yellow ball, purple ball, red ball, white ball, and cyan ball represent Cu, Si, O, H, and H*, respectively. (b) Corresponding CAP dechlorination ratio of CAP on various catalysts after 3 h electrolysis at −1.0 V vs. Ag/AgCl. Reprinted with permission from Ref. [78]. Copyright 2025, John Wiley and Sons. (c) XPS N 1s spectra of TpDz and P-TpDz. (d) Temporal H2O2 generation over TpDz and P-TpDz. (e) Electron spin resonance of O2−. Reprinted with permission from Ref. [79]. Copyright 2025, American Chemical Society.

Fig. 5. (a) Nyquist plots for COF@H3PO4 at different temperatures. (b) Photocatalytic performance of H2O2 production using visible light for different catalysts (10 mg catalyst in 20 mL pure water, λ > 420 nm Xe lamp). (c) Free energy diagram for the two-electron ORR on the COF and COF@H3PO4. (d) The band charge density distributions of the HOMO and LUMO of COF@H3PO4 with an isovalue of 0.0004 e Å-3; the yellow and green colors represent the charge density distribution with and without electron occupation. Reprinted with permission from Ref. [80]. Copyright 2024, American Chemical Society. (e) Mass spectrometry spectra of the hydrogenation product (ethylbenzene) from using H2O or D2O. (f) Schematic illustration of the PWDTH process over the Pt/CN catalyst. Step 1: CN is light excited with the generated electrons transferring to the loaded Pt nanoparticles and holes being captured by scavenger (triethanolamine). Step 2: H2O is reduced to hydrogen (H0) over the Pt nanoparticles. Step 3: Organic molecules containing unsaturated double bonds (C=C, N=O and C=O) are in-situ hydrogenized at the Pt sites. (g) The yield and Apparent Quantum Efficiency (on columns) of the hydrogenation of styrene (C=C), nitrobenzene (N=O) and benzaldehyde (C=O) catalyzed by Pt/CNB and PtPd/CNB; light source: 380 nm LED, 20 mW cm-2. Reprinted with permission from Ref. [82]. Copyright 2020, American Chemical Society.

Fig. 6. (a) Schematic of species transfer governing H2O2 selectivity at the electrode scale. Red and white spheres represent oxygen and hydrogen, respectively. (b) H2O2 production performance of carbon black (CB)/Nafon-thin and CB/PTFE-thin at different current densities in 1 h. Mapping of surface absorbed light intensity (representing OH− concentration) as a function of electrolysis time for hydrophilic CB/Nafion-thin (c) and hydrophobic CB/PTFE-thin (d) at 100 m Acm−2. Reprinted with permission from Ref. [87]. Copyright 2024, Springer Nature. (e) Photocatalytic CO2RR activity and selectivity of Co-NGO under different reaction systems. (f) Plot of ln(c0 - x) and 1/c0 - x vs. time in non-flow system. Reprinted with permission from Ref. [89]. Copyright 2025, John Wiley and Sons.

Fig. 7. (a) Energy-minimized configurations of different proton donors (H2O, NaH2PO4, NaHCO3, and H3BO3 + H2O) adsorption on the (001) surface of Co(OH)2. The ΔEad is the adsorption energy of the proton donors on Co(OH)2. Isosurfaces are 0.03 eV Å-3. (b) Concentration changes of HMF and DHMF in 0.1 mol L-1 phosphate during the chronoamperometry test at 1.2 V vs. Ag/AgCl. (c) The proposed reaction pathway in the real condition of the buffer-promoting electrocatalytic hydrogenation (ECH) process. Reprinted with permission from Ref. [90]. Copyright 2023, Elsevier. (d) Voltage-dependent current density for FA production of the Pt, PtCu0.35, PtCu0.61, PtCu1.29 and Cu electrodes in the MEA systems. (e) Cell voltage profile for the PtCu0.61 MEA system operative at 50 mA cm−2 for 10 h. Reprinted with permission from Ref. [92]. Copyright 2024, American Chemical Society. (f) Reaction profile of PET conversion over dual catalysts of Pd/r-GO and og-CuZn in temperature-programed mode. Reaction conditions: 100 mg PET, 50 mg og-CuZn and 50 mg of Pd/r-GO, 5 mL 1,4dioxane, 120 °C for 4 h, 200 °C for 8 h and 220 °C for 2 h, 6 MPa H2. Reprinted with permission from Ref. [95]. Copyright 2024, John Wiley and Sons.

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Proton hydrogenation reaction in neutral media: Mechanisms, challenges, and performance enhancement strategies

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