Recent advances in hydrogen production using sulfide-based photocatalysts

Dilip Sasmal; Mitali Hupele; Somaditya Sen; Sradhanjali Lenka; Suresh Chandra Baral

REVIEW 3 major objections 8 minor 300 references

Recent advances in hydrogen production using sulfide-based photocatalysts

T0 review · 3 major / 8 minor · reviewed 2026-08-11 · deepseek-v4-flash

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Pith's one-line read This review chapter claims that five modification strategies—heterojunction construction, defect engineering, co-catalyst loading, elemental doping, and single-atom engineering—reliably improve the photocatalytic hydrogen evolution…

desk verdict A broad but uncritical survey; the headline conclusion is not auditable because the compiled HER tables are internally inconsistent. read the letter →

arxiv 2412.05658 v1 pith:PFVAN4B3 submitted 2024-12-07 cond-mat.mtrl-sci

Suresh Chandra Baral , Dilip Sasmal , Mitali Hupele , Sradhanjali Lenka , Somaditya Sen This is my paper · ORCID

classification cond-mat.mtrl-sci

keywords photocatalytichydrogenevolutionmetalsulfidephotocatalystsheterojunctiondefectengineeringco-catalystloadingelementaldopingsingle-atomsolarproduction

verification ladder T0 review T1 audit T2 compute T3 formal

The pith

A machine-rendered reading of the paper's core claim, the machinery that carries it, and where it could break.

The reading

This review chapter tries to establish that sulfide-based photocatalysts, not just cadmium sulfide but a family of binary and ternary metal sulfides, can be made markedly better at splitting water into hydrogen by five modification strategies: heterojunction construction, defect engineering, co-catalyst loading, elemental doping, and single-atom engineering. Its evidence is a compiled survey of recent reports, organized into fifteen tables, showing that modified systems repeatedly outperform pristine sulfides, often by tens to hundreds of times, with the best rates in the hundreds of mmol per gram-hour under visible light. A sympathetic reader should care because sulfide photocatalysts are cheap, visible-light-active alternatives to wide-bandgap oxides, and the review argues that the main obstacles, rapid charge recombination and photocorrosion, are being addressed by these strategies. The chapter closes by acknowledging that performance and stability are still far from industrial requirements and calls for a standard testing protocol, AI/ML-assisted material selection, and scale-up.

What carries the argument

The central object is the modified metal sulfide photocatalyst: a sulfide semiconductor whose electronic structure, charge-carrier dynamics, and surface reactivity are altered by one of five strategies. The mechanism doing most of the work is the heterojunction, especially Type-II, Z-scheme, and S-scheme band arrangements at sulfide interfaces, because it creates internal electric fields that keep photogenerated electrons and holes apart long enough for protons to be reduced. Sulfur vacancies and co-catalysts such as NiS, MoS2, WS2, and FeP supply the active sites and lower the kinetic barriers; elemental doping and single-atom engineering adjust band positions and adsorption energies.

What would settle it

A re-measurement campaign that runs the top tabulated catalysts, for example FeP/CdS at 202 mmol per gram-hour and CdS/WS2-P at 262 mmol per gram-hour, under one identical protocol with the same lamp, intensity, sacrificial reagent, and catalyst loading, and finds rates far below the table values or a different ranking among catalysts, would overturn the claim that these modifications reliably improve performance.

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Extended reading notes

Core claim

The paper's stated conclusion is that the photocatalytic hydrogen evolution performance and stability of metal sulfides are significantly improved after modification using the emerging strategies. The survey covers binary sulfides such as CdS, ZnS, MoS2, WS2, PbS, NiS/NiS2, FeS2, CuS/Cu2S, CoS/CoS2, SnS2, In2S3, and Bi2S3, plus ternary systems such as ZnxCd1-xS, MnxCd1-xS, ZnIn2S4, and CdIn2S4; in each family it finds the same pattern: heterojunctions, sulfur vacancies, co-catalysts, dopants, and single-atom sites increase reported H2 evolution rates and, in many cases, quantum yields. The highest compiled rates reach 202 and 262 mmol per gram-hour for CdS-based systems, and quantum yields in individual reports go as high as 98.4% at 425 nm. The review's own caveat is that these advances remain laboratory-scale and that efficiency and stability are still short of what industry would need.

Load-bearing premise

The load-bearing premise is that the published hydrogen production rates and quantum yields compiled in Tables 1–15 are accurate and comparable across experiments that differ in light source, sacrificial reagent, catalyst loading, and reactor geometry.

Editorial extensions

If this is right

If the compiled numbers are right, the surest route to better sulfide photocatalysts is to combine several strategies at once, since the chapter notes that each modification addresses only part of the photocatalytic process.
Noble-metal-free co-catalysts emerge as a credible substitute for platinum in many tabulated systems, which strengthens the cost argument for solar hydrogen.
The highest reported rates are sufficient that material discovery is no longer the only bottleneck; the chapter's own outlook places reactor design and industrial-scale synthesis on the critical path.
Cadmium-based sulfides dominate the top of the tables, so any practical deployment will have to solve the toxicity and regulation problems the chapter flags, or shift the same strategies onto non-cadmium sulfides.

Reading between the lines

Editorial extensions of the paper, not claims the author makes directly.

Beyond the paper: if a common protocol were adopted, the spread of reported rates would likely narrow, and some fold-improvements in the tables would probably shrink; the rankings by strategy should be read as provisional until then.
Beyond the paper: the stability data in the tables are sparser than the rate data, so the claim that the strategies improve stability is supported more by the qualitative discussion than by the compiled numbers; long-cycle testing is a natural next experiment.
Beyond the paper: the dual-co-catalyst pattern in the best CdS systems, such as NiS-ReS2, Pd+PdS, and MoS2+CoSe2, suggests a testable transfer: applying the same two-co-catalyst logic to less toxic hosts such as ZnIn2S4 or FeS2.

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Editorial analysis

A structured set of objections, weighed in public.

Desk editor's note, referee report, and a circularity audit.

Desk Editor's Note

read the letter

The one thing to know: this is a chapter-length survey, not a research paper. Its value is organizational — a newcomer to sulfide photocatalysis gets a structured map of binary and ternary sulfides, the main modification strategies, and roughly 600 recent references. The writing is clear and the coverage is genuinely broad, and the outlook section makes sensible points about AI/ML screening, cost, and the need for a standard protocol, including a candid acknowledgment of cadmium toxicity. That is real credit, and it is not damning with faint praise. The paper does what a survey should do, at least in scope.

The soft spot is the tabulated evidence. The same Pt-loaded ZnO/ZnS/CdS material appears as 26,400 μmol g−1 h−1 in Table 1 and 2,640 μmol g−1 h−1 in Table 2, both citing reference [161]. A factor-of-ten discrepancy in a flagship entry means the tables cannot be trusted without re-checking every original paper. The problem is not just one typo; the tables mix 300 W Xe lamps, 5 W LEDs, natural sunlight, different sacrificial reagents, loadings, and quantum-yield wavelengths, so cross-row rankings conflate materials with measurement conditions. The stability half of the conclusion is even less supported — there are no cycle counts, retention percentages, or irradiation durations anywhere in the tables. The chapter's own Section 3 calls for a standard protocol, which effectively concedes that the present numbers are not comparable. The general claim that heterojunctions, doping, and co-catalysts help may well be true in the literature, but this chapter does not provide auditable support for it.

There are also presentation issues: two different figures are numbered Figure 4, and Table 8 is used twice (for Cu2S and for CoS/CoS2). These are copyediting problems, not conceptual ones. The author self-citations concern unrelated oxide and perovskite work, but they are not circular because the central claim does not depend on them.

Who is this for? A reader who wants a quick, broad orientation to the field and is willing to go back to the primary literature for numbers. It deserves peer review if the venue has a review track, but only with the expectation of heavy revision: the tables need to be re-verified or explicitly labeled non-comparable, and the conclusion needs to be softened to match what the chapter can actually support.

Referee Report

3 major / 8 minor

Summary. This manuscript is a review chapter surveying recent work on sulfide-based photocatalysts for photocatalytic hydrogen evolution (HER). It covers binary sulfides (CdS, ZnS, MoS2, WS2, PbS, NiS/NiS2, FeS2, CuS/Cu2S, CoS/CoS2, SnS2, In2S3, Bi2S3) and ternary sulfides (ZnxCd1-xS, MnxCd1-xS, ZnIn2S4, CdIn2S4), with fifteen tables of reported H2 evolution rates and quantum yields. The central claim, stated in the conclusion, is that modification strategies—heterojunction construction, defect engineering, cocatalyst loading, elemental doping, and single-atom engineering—significantly improve the photocatalytic HER performance and stability of metal sulfides. The chapter also proposes future directions including AI/ML-guided material selection, a standard measurement protocol, in-situ characterization, and scale-up considerations.

Significance. If its compilation were reliable, the review would be a useful broad survey: it aggregates a large body of literature (about 690 references), covers a wide range of sulfide systems, and explicitly calls for standardization of photocatalytic testing protocols, which is a constructive and needed step for the field. The authors also appropriately flag practical concerns such as the cost of noble metals, cadmium toxicity, and the gap between laboratory rates and industrial requirements. However, the chapter's evidentiary core—the performance tables—contains internal inconsistencies and mixes non-comparable conditions, so the quantitative support for the 'significantly improved' claim is not currently auditable. The review is not machine-checked and adopts record-breaking labels from primary papers without independent verification; it does, however, make its own limitation explicit by recommending a standard protocol. Overall, the review has the potential to be a valuable entry point for researchers if the data compilation is corrected and the stability claim is properly qualified.

major comments (3)

[§2.1.1 Table 1 vs. §2.1.2 Table 2] The same Pt-loaded ZnO/ZnS/CdS photocatalyst, with both entries citing ref. [161], is listed as 26,400 μmol g⁻¹ h⁻¹ in Table 1 and as 2,640 μmol g⁻¹ h⁻¹ in Table 2, a factor-of-ten discrepancy; the text around §2.1.1 reports 26,400 μmol g⁻¹ h⁻¹. Because these tables are the evidentiary basis for the chapter's claim that modification strategies significantly improve HER performance, this internal inconsistency means the compiled dataset cannot be used as a reliable audit trail unless every entry is checked against and corrected from the primary source.
[§4 Conclusion; Tables 1–15] The conclusion states that 'The photocatalytic hydrogen evolution performance and stability of metal sulfides are significantly improved after modification using the emerging strategies,' but the stability half of this claim is not supported by any data in the review: no table reports cycle number, retention percentage, or irradiation duration, and the stability statements in the text (e.g., 'good stability', 'outstanding stability and activity') are qualitative. The chapter should either remove the unsubstantiated stability claim or add quantitative stability metrics if such data are available in the cited primary papers.
[§2, Tables 1–15; §3] The tabulated HER rates are not comparable across rows: light sources range from 300 W Xe lamps to 5 W LEDs and natural sunlight, sacrificial reagents include lactic acid, Na2S/Na2SO3, TEOA, methanol, and ethanol, and catalyst loadings and quantum-yield wavelengths differ widely. As a result, cross-row rankings of 'best' catalysts and the general 'significantly improved' conclusion cannot be audited from the tables alone. Section 3's own call for a 'standard protocol' implicitly concedes this limitation; the text should therefore explicitly state that the compiled rates are raw literature values and should not be compared quantitatively without normalization or stated caveats.

minor comments (8)

[§1, Figures] Figure 4 is numbered twice: once for 'Most employed strategies and representative components' and once for 'The band gap positions of the selected MS semiconductors'; the second figure should be renumbered to avoid ambiguity.
[§2.1.8.2 and §2.1.9, Tables] Table 8 is used twice, first for Cu2S-based photocatalysts and later for CoS/CoS2-based photocatalysts; the later table should be renumbered (e.g., Table 9, with subsequent tables renumbered accordingly).
[§1.1, Equations (2)–(4)] The text cites '[Equation (3)]' for the oxidation potential (+0.82 V) and '[Equation (4)]' for the reduction potential (−0.41 V), but Equations (2) and (3) define the oxidation and reduction half-reactions, respectively; these in-text cross-references should be corrected.
[§2.1] In the list of binary metal sulfides, 'NIS/NiS2' should read 'NiS/NiS2' to match the correct chemical formula.
[§2.1.10] In the description of the SnS2/twinned Mn0.5Cd0.5S hetero-homojunction, '0.24 mmol mmol h⁻¹ g⁻¹' contains a duplicated unit; it should read '0.24 mmol g⁻¹ h⁻¹'.
[Table 10] The table rows labeled 'In,S3–ZnIn2S4/Au' and 'In,S3–ZnIn2S4' contain a typographical error; they should be 'In2S3–ZnIn2S4/Au' and 'In2S3–ZnIn2S4'.
[References] Reference [14] lists the author as 'M. P', which appears to be an incomplete or truncated name; the full author name should be provided.
[§2.1.8.2] The sentence beginning 'Ag2S/Cu2S co-catalysts deposited on CdZnS and observed the 1% Ag2S/Cu2S on CdZnS to produce hydrogen...' is grammatically incomplete and should be revised for clarity.

Circularity Check

0 steps flagged · score 0.0 of 10

No circularity: the chapter is a literature compilation with no derivation chain, and its self-citations are unrelated to the central sulfide-HER claim.

full rationale

The chapter is a review of published experimental results on sulfide-based photocatalysts, not a derivation or prediction from first principles. Its central claim—that heterojunction construction, defect engineering, co-catalyst loading, doping, and single-atom engineering improve photocatalytic hydrogen evolution performance and stability—is an inductive summary of the externally published rates tabulated in Tables 1–15. Each enhancement claim is attributed to independent primary literature (e.g., refs. [113], [121], [125], [126], [129]) with specific H2 evolution activities and quantum yields. The author self-citations ([14]–[22]) concern CuO photocatalysis, La2NiMnO6 double perovskites, and other oxide/perovskite materials; they are not used to justify any sulfide-specific conclusion, so they are not load-bearing. No equation or parameter in the paper is defined in terms of a target result, and no fitted input is renamed as a prediction. The internal inconsistency noted by the reader—the same Pt-loaded ZnO/ZnS/CdS material listed as 26,400 μmol g−1 h−1 in Table 1 and 2,640 μmol g−1 h−1 in Table 2, both citing ref. [161]—is a serious data-quality and comparability problem affecting the auditability of the compiled rates, but it is a correctness and reproducibility concern, not circularity: the conclusion does not reduce by construction to the tabulated numbers. Therefore the circularity score is 0.

Assumptions & free parameters 0 free parameters · 2 assumptions · 0 invented entities

The review's central claim rests on accepting the accuracy and comparability of reported rates from primary papers. No free parameters are introduced because no data fitting or derivation occurs. The main axioms are data-reliability assumptions.

assumptions (2)

domain assumption Reported hydrogen evolution rates and quantum yields in Tables 1-15 are accurate as published and comparable across laboratories.
The central conclusion that modification strategies improve performance depends on comparing rates measured under different light sources, sacrificial reagents, and catalyst loadings without correction.
domain assumption The heterojunction mechanism classifications (type-II, Z-scheme, S-scheme) assigned to each composite in the cited papers are correct.
The review's narrative that these structures improve charge separation relies on accepting the mechanism assignments from the primary literature without independent verification.

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Cite this review

Pith. "Pith review of Recent advances in hydrogen production using sulfide-based photocatalysts." pith.science (2026). https://pith.science/paper/PFVAN4B3

@misc{pith2026241205658,
  author       = {Pith},
  title        = {Pith review of: Recent advances in hydrogen production using sulfide-based photocatalysts},
  year         = {2026},
  howpublished = {\url{https://pith.science/paper/PFVAN4B3}},
  note         = {Machine review of arXiv:2412.05658}
}

read the original abstract

Sulfide-based photocatalysts (PC) are promising materials for efficiently producing hydrogen (H2). This chapter aims to provide a detailed survey of the recent advancements in sulfide-based photocatalysts and emphasize their enhanced performance and pathways to efficient H2 production. A detailed summary has been given, including several metal sulfides, such as cadmium sulfide (CdS), zinc sulfide (ZnS), molybdenum disulfide (MoS2), tungsten disulfide (WS2), lead sulfide (PbS), nickel sulfides (NiS/NiS2), iron disulfide (FeS2), copper sulfides (CuS/Cu2S), cobalt sulfides (CoS/CoS2), tin disulfide (SnS2), indium sulfide (In2S3), bismuth sulfide (Bi2S3), zinc cadmium sulfide (ZnxCd1-xS), manganese cadmium sulfide (MnxCd1-xS), zinc indium sulfide (ZnIn2S4), and cadmium indium sulfide (CdIn2S4). This chapter will focus on the latest advancements in metal-sulfide-based materials for photocatalytic hydrogen evolution reactions (HER), taking its accelerated growth and excellent research into account. After briefly outlining the basic properties, the chapter will showcase the cutting-edge strategies and recent research progress, including the construction of heterojunctions, defect engineering, co-catalyst loading, elemental doping, and single-atom engineering, which improve the electronic structure and charge separation capabilities of metal sulfides for photocatalytic hydrogen production. A future perspective and outlook have been proposed, focusing on some key points and a standard protocol. With this knowledge, we hope sulfide-based photocatalysts can be modified and engineered to improve their efficiency and stability in future research.

Figures

Figures reproduced from arXiv: 2412.05658 by the authors.

**Figure 3.** General requirements for designing highly efficient photocatalysts. [PITH_FULL_IMAGE:figures/full_fig_p007_3.png] view at source ↗

**Figure 4.** Most employed strategies and representative components for enhanced hydrogen production over the MS photocatalysts. The figure covers all the techniques based on recent literature discussed in this review. Furthermore, porous structures have a high Brunauer-Emmett-Teller (BET) surface area and more active sites, facilitating the photocatalytic reaction. Photocatalytic enhancement requires improved solar energy utili… view at source ↗

Figures from the paper (1 more)

**Figure 4.** Figure 4: The band gap positions of the selected MS semiconductors, and the required redox potentials for water splitting. Data obtained from, In2S3 [70], SnS2 [71], ZnIn2S4 [72], MoS2 [73], Bi2S3 [74], CdIn2S4 [75], CuInS2 [76], CdS [77], Cu2ZnSnS4 [78], CuGaS2 [79], CuIn5S8 [8…

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WS2/Graphitic Carbon Nitride Heterojunction Nanosheets Decorated with CdS Quantum Dots for Photocatalytic Hydrogen Production,

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1D/2D CdS/WS2 heterojunction photocatalyst: First- principles insights for hydrogen production,

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Hierarchical Layered WS2/Graphene-Modified CdS Nanorods for Efficient Photocatalytic Hydrogen Evolution,

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Colloidal Synthesis of 1T-WS2 and 2H-WS2 Nanosheets: Applications for Photocatalytic Hydrogen Evolution,

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Harnessing Ti3C2-WS2 nanostructures as efficient energy scaffoldings for photocatalytic hydrogen generation,

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C. Li, X. Zhang, T. Song, Y. Tian, S. Wang, and P. Yang, “Interface-engineering derived WS2/S- g-C3N4 nanosheet Z-scheme heterostructures towards enhanced photocatalytic redox and H2O2 generation,” J. Environ. Chem. Eng., vol. 12, no. 5, p. 113396, Oct. 2024, doi: 10.1016/j.je...

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Enhanced photocatalytic hydrogen production utilizing few-layered 1T-WS2/g-C3N4 heterostructures prepared with one-step calcination route,

R. Cao, H. Yuan, N. Yang, Q. Lu, Y. Xue, and X. Zeng, “Enhanced photocatalytic hydrogen production utilizing few-layered 1T-WS2/g-C3N4 heterostructures prepared with one-step calcination route,” Fuel, vol. 357, p. 129808, Feb. 2024, doi: 10.1016/j.fuel.2023.129808

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Simple synthesis and efficient photocatalytic hydrogen production of WO3-WS2 and WO3–WS2–MoS2,

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Heterostructured WS2- MoS2 Ultrathin Nanosheets Integrated on CdS Nanorods to Promote Charge Separation and Migration and Improve Solar-Driven Photocatalytic Hydrogen Evolution,

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MoSe2-WS2 Nanostructure for an Efficient Hydrogen Generation under White Light LED Irradiation,

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Bacterial synthesis of PbS nanocrystallites in one- step with l-cysteine serving as both sulfur source and capping ligand,

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PbS-sensitized K2Ti4O9 composite: Preparation and photocatalytic properties for hydrogen evolution under visible light irradiation,

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Synthesis and characterization of PbS/ZnO thin film for photocatalytic hydrogen production,

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Electronic Structure Reconfiguration toward Pyrite NiS2 via Engineered Heteroatom Defect Boosting Overall Water Splitting,

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Multi-walled carbon nanotubes with embedded nickel sulphide as an effective electrocatalyst for Bi-functional water splitting,

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Constructing Multifunctional Metallic Ni Interface Layers in the g-C3N4 Nanosheets/Amorphous NiS Heterojunctions for Efficient Photocatalytic H2 Generation,

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One-pot hydrothermal synthesis of CdS/NiS photocatalysts for high H2 evolution from water under visible light,

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Highly efficient and noble metal-free NiS modified MnxCd1-xS solid solutions with enhanced photocatalytic activity for hydrogen evolution under visible light irradiation,

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CuS, NiS as co-catalyst for enhanced photocatalytic hydrogen evolution over TiO2,

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Sulfur-mediated photodeposition synthesis of NiS cocatalyst for boosting H2-evolution performance of g-C3N4 photocatalyst,

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Noble-Metal-Free NiS/C3N4 for Efficient Photocatalytic Hydrogen Evolution from Water,

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Au NPs-incorporated NiS/RGO hybrid composites for efficient visible light photocatalytic hydrogen evolution,

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Highly efficient and noble metal-free NiS/CdS photocatalysts for H 2 evolution from lactic acid sacrificial solution under visible light,

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Strong interfacial coupling for NiS thin layer covered CdS nanorods with highly efficient photocatalytic hydrogen production,

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NiS-Decorated ZnO/ZnS Nanorod Heterostructures for Enhanced Photocatalytic Hydrogen Production: Insight into the Role of NiS,

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Photodeposition of NiS thin film enhanced the visible light hydrogen evolution performance of CdS nanoflowers,

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Extended visible to near-infrared harvesting of earth-abundant FeS2–TiO2 heterostructures for highly active photocatalytic hydrogen evolution,

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Pyrite FeS2 nanostructures: Synthesis, properties and applications,

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Modification, application and reaction mechanisms of nano-sized iron sulfide particles for pollutant removal from soil and water: A review,

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Iron Sulfide Materials: Catalysts for Electrochemical Hydrogen Evolution,

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Pith tools

Reviewed August 11, 2026 · model on record in the stance chip above.

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