Highest Hydrogen Evolution Rate Research Articles

Enhancing photocatalytic hydrogen production in conjugated porous polymers through donor-π-donor fragment insertion

Recent progress in conjugated polymer photocatalysts has opened avenues for enhancing photocatalytic hydrogen production (PHP) activity through structural design. This study highlights the impact of the acceptor-to-donor feed ratio on PHP activity in copolymers, influencing their energy level structures. Five conjugated porous polymers (CPPs) were synthesized by adjusting the acceptor-to-donor molar ratio. Notably, at a 2:1 acceptor-to-donor ratio, the polymer demonstrated a high hydrogen evolution rate (HER) of 61.9 mmol g−1 h−1 under full arc irradiation without co-catalysts and an apparent quantum yield (AQY) of 7.77% at 475 nm. However, further increasing the proportion of the donor unit in the copolymers decreases their HER. Experiments and theoretical simulation characterized that the feed ratios effectively tune the polymer's molecular structure, hydrophilicity, band gap, and the generation and transport efficiency of photo-induced charge carriers, ultimately affecting the hydrogen production kinetics and efficiency. This research demonstrates that tuning the band structure and chemical compositions of CPPs through statistical copolymerization significantly impacts their PHP activity.

Enhancing photocatalytic hydrogen production in conjugated porous polymers through donor-π-donor fragment insertion

Recent progress in conjugated polymer photocatalysts has opened avenues for enhancing photocatalytic hydrogen production (PHP) activity through structural design. This study highlights the impact of the acceptor-to-donor feed ratio on PHP activity in copolymers, influencing their energy level structures. Five conjugated porous polymers (CPPs) were synthesized by adjusting the acceptor-to-donor molar ratio. Notably, at a 2:1 acceptor-to-donor ratio, the polymer demonstrated a high hydrogen evolution rate (HER) of 61.9 mmol g−1 h−1 under full arc irradiation without co-catalysts and an apparent quantum yield (AQY) of 7.77% at 475 nm. However, further increasing the proportion of the donor unit in the copolymers decreases their HER. Experiments and theoretical simulation characterized that the feed ratios effectively tune the polymer's molecular structure, hydrophilicity, band gap, and the generation and transport efficiency of photo-induced charge carriers, ultimately affecting the hydrogen production kinetics and efficiency. This research demonstrates that tuning the band structure and chemical compositions of CPPs through statistical copolymerization significantly impacts their PHP activity.

Stable Pt/MgAl2O4 catalysts for efficient production of H2 from cyclohexane dehydrogenation

Cyclohexane as liquid organic hydrogen carriers has attracted considerable interest in the field of hydrogen storage technology. However, the innovation of efficient catalyst for producing H2 through cyclohexane dehydrogenation remains a substantial challenge. In this study, we have successfully developed Pt/MgAl2O4 catalysts exhibiting outstanding catalytic performance in cyclohexane dehydrogenation. Notably, the optimal catalyst Pt/MgAl2O4-700 achieves cyclohexane conversion of 89.1 % and benzene selectivity of over 99 % at 345 °C, resulting in a high hydrogen evolution rate of 933 mmol/gPt/min. Moreover, this catalyst exhibits remarkable long-term stability, with no evident loss of activity in 225-hour dehydrogenation reaction. The catalyst was characterized by XRD, N2 adsorption–desorption, STEM, XPS, NH3-TPD, CO-FTIR and H2-TPR techniques, which provides detailed structure information for elucidation of structure–activity relationship. The spinel structure and moderate acid density of the support enable highly dispersed Pt species at the surface of MgAl2O4. This results in the formation of ultra-small and sintering-resistant Pt particles that exhibit exceptional activity in cyclohexane dehydrogenation. Additionally, the presence of positively charged Ptδ+ species in Pt/MgAl2O4 facilitates the rapid desorption of benzene product. This effectively prevents the formation of coke arising from benzene dehydrogenation, which ensures to achieve high stability. These findings provide valuable knowledge for the rational design of efficient metal-based catalysts for liquid organic hydrogen carriers in hydrogen storage systems.

One step co-deposition of Ni0.96S and Ag2S on TiO2 nanosheets for enhanced photocatalytic H2 generation with superior stability

Introduction of co-catalysts to construct heterojunctions is one of the important strategies to improve the photocatalytic hydrogen production activity of semiconductor catalysts. Here, Ni0.96S and Ag2S co-decorated TiO2 composites were prepared by a simple one-step solvothermal method, whose photocatalytic H2 production activities were evaluated and related H2 evolution mechanism was explored. The 5%Ni0.96S-8%Ag2S/TiO2 ternary composite exhibited much enhanced photocatalytic activity with the photocatalytic hydrogen evolution rate (HER) of 23.67 mmol·h−1·g−1, which is 131.5 fold higher than that of the pure TiO2. Even higher HER, 29.45 mmol·h−1·g−1, was obtained in the presence of 40 mL glycerol. The photocatalytic HERs of the 5%Ni0.96S-8%Ag2S/TiO2 catalyst under visible light (λ > 420 nm) and simulated solar light (AM1.5) were 353.78 and 935.24 µmol·h−1·g−1, respectively. The apparent quantum efficiency (365 nm) is as high as 13.9%. Remarkably, the catalyst exhibited excellent photocatalytic cycling stability and durability, beneficial to practice applications. The improved photocatalytic activity of the composite can be attributed to much improved charge carrier transfer/separation, optimized energy band structure and enhanced visible light absorption caused by synergistic effect of Ni0.96S and Ag2S.

Symmetry‐breaking of Dibenzo[b,d]thiophene Sulfone Enhancing Polaron Generation for Boosted Photocatalytic Hydrogen Evolution

AbstractThe current bottleneck in the development of efficient photocatalysts for hydrogen evolution is the limited availability of high‐performance acceptor units. Over the past nine years, dibenzo[b,d]thiophene sulfone (DBS) has been the preferred choice for the acceptor unit. Despite extensive exploration of alternative structures as potential replacements for DBS, a superior substitute remains elusive. In this study, a symmetry‐breaking strategy was employed on DBS to develop a novel acceptor unit, BBTT‐1SO. The asymmetric structure of BBTT‐1SO proved beneficial for increasing multiple moment and polarizability. BBTT‐1SO‐containing polymers showed higher efficiencies for hydrogen evolution than their DBS‐containing counterparts by up to 166 %. PBBTT‐1SO exhibited an excellent hydrogen evolution rate (HER) of 222.03 mmol g−1 h−1 and an apparent quantum yield of 27.5 % at 500 nm. Transient spectroscopic studies indicated that the BBTT‐1SO‐based polymers facilitated electron polaron formation, which explains their superior HERs. PBBTT‐1SO also showed 14 % higher HER in natural seawater splitting than that in deionized water splitting. Molecular dynamics simulations highlighted the enhanced water‐PBBTT‐1SO polymer interactions in salt‐containing solutions. This study presents a pioneering example of a substitute acceptor unit for DBS in the construction of high‐performance photocatalysts for hydrogen evolution.

Symmetry-breaking of Dibenzo[b,d]thiophene Sulfone Enhancing Polaron Generation for Boosted Photocatalytic Hydrogen Evolution.

The current bottleneck in the development of efficient photocatalysts for hydrogen evolution is the limited availability of high-performance acceptor units. Over the past nine years, dibenzo[b,d]thiophene sulfone (DBS) has been the preferred choice for the acceptor unit. Despite extensive exploration of alternative structures as potential replacements for DBS, a superior substitute remains elusive. In this study, a symmetry-breaking strategy was employed on DBS to develop a novel acceptor unit, BBTT-1SO. The asymmetric structure of BBTT-1SO proved beneficial for increasing multiple moment and polarizability. BBTT-1SO-containing polymers showed higher efficiencies for hydrogen evolution than their DBS-containing counterparts by up to 166 %. PBBTT-1SO exhibited an excellent hydrogen evolution rate (HER) of 222.03 mmol g-1 h-1 and an apparent quantum yield of 27.5 % at 500 nm. Transient spectroscopic studies indicated that the BBTT-1SO-based polymers facilitated electron polaron formation, which explains their superior HERs. PBBTT-1SO also showed 14 % higher HER in natural seawater splitting than that in deionized water splitting. Molecular dynamics simulations highlighted the enhanced water-PBBTT-1SO polymer interactions in salt-containing solutions. This study presents a pioneering example of a substitute acceptor unit for DBS in the construction of high-performance photocatalysts for hydrogen evolution.

Effect of barnacle on the cathodic protection of high-strength steel and its potential risk related to hydrogen permeation

The cathodic protection efficiency and hydrogen permeation behaviour of high-strength steel with barnacle adhesion in the tidal zone were studied using field exposure and laboratory simulation tests for 2 years. Because of the shielding effect, barnacles can lead to an uneven calcareous deposition, a flatter morphology and a higher protection efficiency of steel. By contrast, because of the higher hydrogen permeation current at the edge of the barnacle adhesion area (caused by a higher hydrogen evolution rate), barnacle adhesion can promote hydrogen permeation. A mechanism was proposed to explain the observed phenomenon, and its effect on service safety was analysed.

Rechargeable zinc-water battery for sustainable hydrogen generation

Metal-water primary batteries hold promise for distributed hydrogen production but suffer from limited renewability of metal electrodes in aqueous electrolytes. Here, we introduce a novel concept of a rechargeable zinc-water battery featuring a reversible zinc anode paired with a bifunctional water electrolysis electrode, realized in a specially designed aqueous electrolyte-a mild zinc triflate aqueous electrolyte with the addition of ethylenediaminetetraacetic acid disodium (EDTANa2). The system enables high-purity hydrogen production during discharge and high-purity oxygen production during charge in a membrane-free setup. In the zinc-water battery, EDTANa2 enhances the water-splitting electrode's performance by replacing hydrophobic OTF- anions, ensuring optimal water activity. Additionally, EDTANa2 enhances Zn electrode reversibility by chelating Zn2+, preventing solvated water decomposition during zinc deposition. This integrated battery continuously undergoes charge-discharge cycles for over 55 h at a current density of 6 mA cm-2. Moreover, it achieves a high hydrogen evolution rate of 12.5 mL cm-2 h-1, enabling cost-effective, high-purity hydrogen production without expensive membranes. These findings open new avenues for sustainable hydrogen generation and energy storage in nano energy systems.

Ti3C2 MXene flakes assisted Mn0.5Cd0.5S/Ti3C2 MXene/g-C3N4 Z-scheme heterojunction for enhancing photocatalytic hydrogen evolution

Efficient carrier separation and high electron migration efficiency are essential for sustainable H2 energy production via photocatalysis. In this work, a Mn0.5Cd0.5S/Ti3C2 MXene/g-C3N4 all-solid-state Z-scheme photocatalyst is constructed by a series of processes, including low temperature calcination, etching, ultrasonication and solvothermal process. The appropriate energy band structures of g-C3N4 and Mn0.5Cd0.5S enable the formation of the Z-scheme system, achieving efficient carrier separation. The Ti3C2 MXene flakes assembled between g-C3N4 nanosheets and Mn0.5Cd0.5S particles can accelerate the charge migration rate in the system. The optimized ternary composite exhibits the highest hydrogen evolution rate (HER) of 13.7 mmol g−1 h−1, which is much higher than that of the pure g-C3N4 and Mn0.5Cd0.5S. Meanwhile, the apparent quantum yield (AQY) value of the composite at 420 nm reaches up to 24.07 % and exhibits high stability. Based on the characterization, the photocatalytic mechanism of carrier transfer in the Z-scheme heterojunction is also revealed. The finding of this article provides insights into the high efficiency of carrier transfer and separation in the photocatalytic reactions.

Optimized synthesis of Fe-doped Ohmic Schottky heterojunctions for efficient NO3− photocatalytic reduction to generate N2

Capacitive Fe-doped Ni2P(Fe2xNi2(1-x)P) is synthesized via the modified solvothermal method to form Ohmic Schottky heterojunctions with monolayer Ti3C2 (MLTC). The composite (10 % 0.1FNP/CdS-2 % MLTC) achieved a high hydrogen evolution rate (HER) of 19.18 mmol·h−1 with a 50 mg sample. In a mere span of 3 h, an impressive NO3− reduction of 0.42 mg/L was achieved, accompanied by an exceptional 92 % N2 selectivity. Quantum efficiency (QE) can reach 56.22 % (λ = 475 nm) by adding 0.1FNP and MLTC. In contrast to previous catalysts, the QE of visible light after 500 nm has been improved to 45.2 % (λ = 500 nm) or 36.4 % (λ = 550 nm). The significant enhancement of HER and NO3− reduction is attributed to the enhanced adsorption of oxygen-containing reactants, the lowering of the reduction overpotential, further enhanced separation efficiency of photogenerated carriers through the ohmic Schottky heterojunction after iron doping. Additionally, the observed capacitor-like nature of 0.1FNP is also an essential factor for the enhanced reduction ability of the composites.

Optimizing Electronic Density at Active W Sites for Boosting Photocatalytic H2 Evolution.

It is highly desirable but challenging to optimize the electronic structure of an active site to realize moderate active site-Hads bond energies for boosting photocatalytic H2 evolution. Herein, an interfacial engineering strategy is developed to simultaneously concentrate hydrogen species and accelerate the combination of an Hads intermediate to generate free H2 by constructing W-WC-W2C (WCC) cocatalysts. Systematic investigations reveal that hybridizing with W2C creates electron-rich W active sites and effectively induces the downshift of the d-band center of W in WC. Consequently, the strong W-Hads bonds on the surface of WC are weakened, thus promoting the desorption of Hads to rapidly produce free H2. The optimized 40-WCC/CdS photocatalyst exhibits a high hydrogen evolution rate of 63.6 mmol g-1 h-1 under visible light (≥420 nm) with an apparent quantum efficiency of 39.5% at 425 nm monochromatic light, which is about 40-fold of the pristine CdS. This work offers insights into the design of cocatalyst for high-efficiency photocatalytic H2 production.

Screening potential dye sensitizers for water splitting photocatalysts using a genetic algorithm.

Addressing the global fossil energy crisis necessitates the efficient utilization of sustainable energy sources. Hydrogen, a green fuel, can be generated using sunlight, water, and a photocatalyst. Employing sensitizers holds promise for enhancing photocatalyst performance, enabling high rates of hydrogen evolution through increased visible light absorption. However, sifting through millions of diverse molecules to identify suitable dyes for specific photocatalysts poses a significant challenge. In this study, we integrate genetic algorithm and geometry-frequency-noncovalent extended tight binding methods to efficiently screen 2.6 million potential sensitizers with a D-π-A-π-AA structure within a short timeframe. Subsequently, these optimized sensitizers are rigorously reassessed by using DFT/TDDFT methods, elucidating why they may serve as superior dyes compared to the reference dye WS5F, particularly in terms of light absorption, driving force, binding energy, etc. Additionally, our methodology uncovers molecular motifs of particular interest, including the furan π-bridge and the double cyano anchoring acceptor, which are prevalent in the most promising set of molecules. The developed genetic algorithm workflow and dye design principles can be extended to various compelling projects, such as dye-sensitized solar cells, organic photovoltaics, photo-induced redox reactions, pharmaceuticals, and beyond.

Photothermally driven decoupling of gas evolution at the solid-liquid interface for boosted photocatalytic hydrogen production.

The slow mass transfer, especially the gas evolution process at the solid-liquid interface in photocatalytic water splitting, restricts the overall efficiency of the hydrogen evolution reaction. Here, we report a novel gas-solid photocatalytic reaction system by decoupling hydrogen generation from a traditional solid-liquid interface. The success relies on annealing commercial melamine sponge (AMS) for effective photothermal conversion that leads to rapid water evaporation. The vapor flows towards the photocatalyst covering the surface of the AMS and is split by the catalyst therein. This liquid-gas/gas-solid coupling system avoids the formation of photocatalytic bubbles at the solid-liquid interface, leading to significantly improved mass transfer and conversion. Utilizing CdS nanorods anchored by highly dispersed nickel atoms/clusters as a model photocatalyst, the highest hydrogen evolution rate from water splitting reaches 686.39 μmol h-1, which is 5.31 times that of the traditional solid-liquid-gas triphase system. The solar-to-hydrogen (STH) efficiency can be up to 2.06%. This study provides a new idea for the design and construction of efficient practical photocatalytic systems.

Recent Progress and Challenges in Perylene Small Molecules, Assemblies and Composites for Photocatalytic Hydrogen Evolution

AbstractPerylene diimide (PDI) derivatives are among the best‐known n‐type organic semiconductors because of their unique photophysical and chemical characteristics. In recent years, significant progress has been made in the development of various PDI/composites and their self‐assembled structures for photocatalytic hydrogen (H2) evolution. However, the slow transport of photogenerated charge carriers, rapid charge recombination, limited catalytic activity, and instability of these materials still pose difficulties for their practical use. In order to address these problems, extensive studies have been conducted on structural modifications, molecular design, and synthesis techniques to control the morphology of self‐assembled PDI structures and create new and effective photocatalysts. In this context, perylene based small molecules, their composites with TiO2 and g‐C3N4, self‐assembled perylene derivatives have been designed and their roles as heterogenous photocatalysts for H2 evolution have been investigated thoroughly in literature. In this review, the developments of PDI‐based photocatalysts for H2 evolution are outlined under four different categories. Self‐assembled PDI nanostructures have made the most advancements among all the categories, with highest hydrogen evolution rate (HER) of 61.49 mmol g−1 h−1 while composites composed of perylene derivatives and g‐C3N4 exhibited the second highest rate of hydrogen evolution (17.7 mmol g−1 h−1). This review is intended to give researchers a better understanding and guidelines for designing PDI‐based and other chromophore‐based materials for efficient H2 evolution and their further exploration for future improvement in H2 evolution efficiencies.

Donor-acceptor moiety functionalized covalent organic frameworks for boosting charge separation and H2 photogeneration

Covalent organic frameworks (COFs) have a broad prospect to be used as a photocatalytic platform to convert solar energy into valuable chemicals due to their tunable structures and rich active catalytic sites. However, constructing COFs with tuned sp2-carbon donor-acceptor moiety remains an enormous challenge. Herein, we synthesized two new fully π-conjugated cyano-ethylene-linked COFs containing benzotrithiophene as functional group by Knoevenagel polycondensation reaction. The accetpor 2,2′-bipyridine unit in BTT-BpyDAN-COF skeleton favored the formation of a intermolecular specific electron transport pathway with the donor benzotrithiophene, and thereby promoted charge separation and transfer efficiency. Specifically, a donor-acceptor (D-A) type BTT-BpyDAN-COF exhibited high hydrogen evolution rate of 10.1 mmol g-1h−1 and an excellent apparent quantum efficiency of 4.83 % under visible light irradiation.

Rational design of pyrene and thienyltriazine-based conjugated microporous polymers for high-performance energy storage and visible-light photocatalytic hydrogen evolution from water

Conjugated microporous polymers (CMPs) have found extensive applications in various fields such as optoelectronics, CO2 capture, and catalysis. However, their potential in electrochemical supercapacitors as energy storage and H2 production systems remains relatively unexplored. This limited exploration can be attributed to certain challenges, including issues related to structural and electrochemical stability, as well as the relatively modest specific capacitance. Additionally, many of the CMPs discovered thus far have exhibited lower energy densities, further contributing to this underexplored aspect of their utility. In this study, we prepared two different CMPs [TPET-TTh and PyT-TTh CMPs] containing thienyltriazine units (TTh) for the redox mechanism and constructed electrodes for supercapacitor applications. The synthesized TPET-TTh and PyT-TTh CMPs displayed exceptionally high specific surface areas of 545 and 528 m² g⁻¹, respectively. Furthermore, their pore sizes were very similar, centered at approximately 0.39 and 0.36 nm, respectively. To evaluate their electrochemical properties, the TTh-CMPs were examined using cyclic voltammetry (CV) and galvanostatic charge/discharge (GCD). The resulting CV curves exhibited rectangular shapes, indicative of the characteristic behavior of electric double-layer capacitors, across a range of potential and scan rates. These TPET-TTh and PyT-TTh CMPs delivered nominal specific capacitances of 74 and 76 F g−1 at 0.5 A g−1, respectively. In addition, they exhibited outstanding capacity retentions of 95.2 and 97.30 % even after 2000 cycles [analyzed at 10 A g−1]. The TTh-CMPs also exhibited excellent light-capture capabilities. The PyT-TTh CMP has faster charge separation and lower charge recombination rates than TPET-TTh CMP. This results in a higher hydrogen evolution rate from the water decomposition reaction. The H2 production rate of PyT-TTh CMP could be as high as 18,533 μmol g−1 h−1, which is approximately 4-fold that of TPET-TTh CMP. This study offers a strategy for the design of TTh-containing CMPs that exhibit exceptional energy storage application and photocatalytic efficiency for H2 evolution.

Oligo(phenylenevinylene)-Based Covalent Organic Frameworks with Kagome Lattice for Boosting Photocatalytic Hydrogen Evolution.

Covalent organic frameworks (COFs) have shown great advantages as photocatalysts for hydrogen evolution. However, the effect of linkage geometry and type of linkage on the extent of π-electron conjugation in the plane of the framework and photocatalytic properties of COFs remains a significant challenge. Herein, two Kagome (kgm) topologic oligo(phenylenevinylene)-based COFs are designed and synthesized for boosting photocatalytic hydrogen evolution via a "two in one" strategy. Under visible light irradiation, COF-954 with 5 wt% Pt as cocatalyst exhibits high hydrogen evolution rate (HER) of 137.23mmol g-1 h-1 , outperforming most reported COF-based photocatalysts. More importantly, even in natural seawater, COF-954 shows an average HER of 191.70mmol g-1 h-1 under ultraviolet-visible (UV-vis) light irradiation. Additionally, the water-drainage experiments indoors and outdoors demonstrate that 25 and 8mL hydrogen gas could be produced in 80 min under UV-vis light and natural sunlight, respectively, corresponding to a high HER of 167.41 and 53.57mmol h-1 g-1 . This work not only demonstrates an effective design strategy toward highly efficient COF-based photocatalysts, but also shows the great potential of using the COF-based photocatalysts for photocatalytic hydrogen evolution.

Direct C-H Arylation Derived Ternary D-A Conjugated Polymers: Effects of Monomer Geometries, D/A Ratios, and Alkyl Side Chains on Photocatalytic Hydrogen Production and Pollutant Degradation.

Donor-acceptor (D-A) conjugated polymer (CP) featuring high charge mobility and widely tunable energy bands have shown promising prospects in photocatalysis. In this work, a library of ternary D-A CPs (22 polymers) based on benzothiadiazole, bithiophene, and fluorene derivatives (i.e., fluorene [Fl], 9,9-dihexylfluorene [HF], and 9,9'-spirobifluorene [SF]) with and without alkyl side chains, and with 3D geometry are designed and synthesized via atom-economical direct C-H arylation polymerization to explore the synergetic effects of stereochemistry, D/A ratio, and alkyl chains on the properties and photocatalytic performances, which reveal that 1) the cross-shaped 3D spirobifluorene (SF) building block shows the highest hydrogen evolution rates (HER) owing to the sufficient photocatalytic active sites exposed, 2) the alkyl-free linear polymer (FlBtBT0.05 ) exhibit the highest photocatalytic pollutant degradation performance owing to its superior charge separation, and 3) the alkyl side chains are redundances that will exert detrimental effects on the aqueous photocatalysis owing to their insulating and hydrophobic property. The structure-property-performance correlation results obtained will provide a desirable guideline for the rational design of CP-based photocatalysts.

Synergistic enhancement of photocatalytic hydrogen evolution by ultrathin oxygen-doped graphitic carbon nitride nanosheets loaded amorphous mesoporous nickel hydroxide

Graphitic carbon nitride (g-C3N4, CN) is widely utilized in the field of photocatalytic hydrogen production owing to its exceptional visible light absorption, addressing the challenge of energy scarcity. However, its development has been hindered by the issue of low charge separation efficiency. In this study, an ultrathin (∼1.65 nm) oxygen-doped graphitic carbon nitride nanosheets loaded amorphous mesoporous nickel hydroxide (a-Ni(OH)2/OCN) photocatalyst was developed through a straightforward calcination and stirring approach. Under visible light irradiation, a-Ni(OH)2/OCN exhibited a remarkably high photocatalytic hydrogen evolution rate of 4764.9 μmol·h−1 g−1, which is 4.7 times greater than that of the original CN. The synergistic effect between O-doping and heterojunction was proved by experimental data analysis combined with DFT calculations. Totally, the introduction of oxygen into CN led to a reduction in its band gap, while a-Ni(OH)2/OCN heterojunction achieved a broaden light absorption range and an effective charge separation due to a type-Ⅱ internal electric fields.

One-pot synthesis of a CdS–MoS2 / CNTs nano-composite for photocatalytic hydrogen production under visible light

The need to meet growing energy demands of global society in a sustainable fashion requires the development of techniques and processes to reduce dependence on fossil fuels and transit to renewable energy sources. Environmentally benign technologies for alternative fuel production in the form of hydrogen can be developed via heterogenous photocatalysis, a process based on utilization of solar energy. To this end, a cadmium sulfide (CdS) based photocatalyst was developed, doped with MoS2 in a one-pot solvothermal synthesis technique, and coupled with multi-walled carbon nanotubes (MWCNTs) as a carbonaceous support. The material exhibiting the highest rate of hydrogen evolution, CM5C3, involved a MWCNTs loading of 3% and MoS2 loading of 5%. Compared to pure CdS synthesized with the same adapted procedure, the 3% CNT loading improved the rate of hydrogen production by nearly 7-fold, and the optimal 5% MoS2 loading further improved the performance by 60%. CM5C3, achieved an apparent quantum efficiency of 7.34%, a 26-fold increase compared to pure CdS. FESEM and HRTEM imaging confirmed the nanorod-like growth of CdS–MoS2 on the CNT surface, with elemental mapping confirming homogenous dispersion of MoS2 and CNTs. In addition, lattice fringe spacings indicated the presence of cubic and hexagonal CdS growing predominantly along the (111) and (002) planes respectively, in addition to MoS2 distributed throughout the crystal lattice. XRD analysis confirmed the presence of hexagonal and cubic CdS, however, MoS2 phases were not registered perhaps due to the low concentration present in the bulk of the material. XPS survey scans showed the presence of C, Cd, Mo, and S only, with trace oxygen impurities. Peak deconvolution indicated the presence of characteristic peaks for CdS and MoS2, in addition to evidence of the presence of Cd–C bonds, indicating strong CdS heterojunctions to the CNT surface.