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Electrochemical catalysts for the hydrogen evolution reaction (HER) have attracted increasing attentions. Noble metal-free cocatalysts play a vital role in HER applications. Herein, a novel strategy to prepare a Ni2P/MoS2 cocatalyst through a simple hydrothermal-phosphorization method was reported, and the prepared cocatalyst was then loaded on an N-doped carbon substrate with excellent conductive performance. The large surface area of the carbon substrate provided many active sites, and the interface between Ni2P and MoS2 improved the catalytic performance for the HER. Compared with pure Ni2P catalyst and MoS2 catalyst, the prepared Ni2P/MoS2 cocatalyst exhibited enhanced catalytic performance. In addition, the results indicate that the prepared cocatalyst has a wide pH range and low onset potential values of 280, 350 and 40 mV in acidic, phosphate-buffered saline and alkaline solutions, respectively, and the corresponding Tafel slopes are 75, 121 and 95 mV dec−1, respectively. Density functional theory (DFT) was adopted to calculate the hydrogen adsorption free energy (△GH∗). The results showed that the interface between Ni2P and MoS2 reduced △GH∗, which was beneficial to the adsorption of hydrogen. Present preparation of cocatalysts with unique interfaces provides a new strategy for improving the catalytic performance of HER.

Judiciously engineering the electrocatalysts is attractive and challenging to exploit materials with high electrocatalytic performance for hydrogen evolution reaction. Herein, we successfully perform the interface engineering by alternately depositing Co-P and Ni-Fe-P films on nickel foam, via facile electroless plating and de-alloying process. This work shows that there is a significant effect of de-alloying process on alloy growth. The electronic structure of layered alloys is improved by interface engineering. The multilayer strategy significantly promotes the charge transfer. Importantly, the Co-P/Ni-Fe-P/NF electrode fabricated by interface engineering exhibits excellent electrocatalytic hydrogen evolution activity with an overpotential of 43.4 mV at 10 mA cm-2 and long-term durability for 72 h in alkaline medium (1 M KOH). The innovative strategy of this work may aid further development of commercial electrocatalysts.

Featured with high power density, improved safety and low-cost, rechargeable aqueous zinc-ion batteries (ZIBs) have been revived as possible candidates for sustainable energy storage systems in recent years. However, the challenges inherent in zinc (Zn) anode, namely dendrite formation and interfacial parasitic reactions, have greatly impeded their practical application. Whereas the critical issue of dendrite formation has attracted widespread concern, the parasitic reactions of Zn anodes with mildly acidic electrolytes have received very little attentions. Considering that the low Zn reversibility that stems from interfacial parasitic reactions is the major obstacle to the commercialization of ZIBs, thorough understanding of these side reactions and the development of correlative inhibition strategies are significant. Therefore, in this review, the brief fundamentals of corrosion and hydrogen evolution reactions at Zn surface is presented. In addition, recent advances and research efforts addressing detrimental side reactions are reviewed from the perspective of electrode design, electrode–electrolyte interfacial engineering and electrolyte modification. To facilitate the future researches on this aspect, perspectives and suggestions for relevant investigations are provided lastly.

The design of efficient, stable, and economical electrocatalysts for oxygen and hydrogen evolution reaction (OER and HER) is a major challenge for overall water splitting. Herein, a hierarchical structured CoP/carbon nanofibers (CNFs) composite was successfully synthesized and its potential application as a high-efficiency bifunctional electrocatalyst for overall splitting water was evaluated. The synergetic effect of two-dimensional (2D) CoP nanosheets and one-dimensional (1D) CNFs endowed the CoP/CNFs composites with abundant active sites and rapid electron and mass transport pathways, and thereby significantly improved the electrocatalytic performances. The optimized CoP/CNFs delivered a current density of 10 mA cm−2 at low overpotential of 325 mV for OER and 225 mV for HER. In the overall water splitting, CoP/CNFs achieved a low potential of 1.65 V at 10 mA cm−2. The facile strategy provided in the present work can facilitate the design and development of multifunctional non-noble metal catalysts for energy applications.

Electrocatalytic water splitting using power generated from renewable energy to produce hydrogen has been considered as one of the more attractive approach to alleviate the problems of energy crisis and environmental pollution. One of the biggest challenges for the large-scale application of water electrolysis is the searching of the low cost electrocatalysts with high and stable activity toward both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). The well-developed porous features of materials synthesized from the earth abundant elements endow them with the enhanced mass transfer and improved electronic interconnection during electrochemical reactions, resulting in the excellent electrocatalytic performance for both OER and HER. Herein, this review focuses on the recent development of innovation strategies for the fabrication of porous non-noble-metal materials including heteroatom-doped carbon-based and transition metal (mainly Co, Ni, and Fe)-based materials as efficient electrocatalysts for overall water splitting. Specially, a detailed discussion of the structure–activity correlation gives an insight on the origin of the high electrocatalytic performance of porous materials obtained from different strategies, and provides guidance for future design and preparation of highly efficient electocatalysts based on non-precious carbon or metal materials for overall water splitting.

Pt-based materials are the state-of-the-art catalysts for hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR); however, there is still much room to improve the catalytic activity and enhance the stability of Pt-based catalysts. In this work, two-dimensional (2D) graphdiyne (GDY) with uniform distributed pores was applied to cover the Pt surface for catalyzing HER and ORR through density functional theory (DFT) calculations. The 2D confinement induced by GDY was found to improve the catalytic performance of the Pt catalyst from three aspects: (1) the 2D covering layer increases the stability of the Pt catalyst through forming the heterogeneous interface of GDY/Pt(111); (2) GDY/Pt(111) shows better catalytic activities of HER and ORR, with the smaller average overpotential values of 0.26 and 0.51 V, respectively, compared with those (0.29 V for HER, 0.62 V for ORR) on the Pt catalyst; (3) the confinement effect of GDY weakens the adsorption energy of CO to -1.81 eV (average value) from -2.14 eV on Pt(111), inhibiting CO poisoning. This work sheds new light on 2D confinement effects for HER and ORR, which opens up a new strategy for improving the catalytic performance of Pt-based catalysts.

Hydrogen production by water electrolysis is a compelling technology to produce fuels and chemicals powered by renewable energy. It is highly desirable to develop cost-effective and durable electrocatalysts for hydrogen evolution reaction (HER). This review has summarized recent progress in mechanism understanding of non-precious metal electrocatalysts for pH-universal HER. The general approaches have been demonstrated to overcome the activity/stability limitations of the electrocatalysts for HER in a broad pH range. The perspectives and challenges for the development of pH-universal HER electrocatalysts have also been proposed. This review sheds light on the design and fabrication of high-performance electrocatalysts for versatile HER-related energy technologies.

Development of high-performance and cost-effective catalysts for electrocatalytic hydrogen evolution reaction (HER) play crucial role in the growing hydrogen economy. Recently, the atomically dispersed metal catalysts have attracted increasing attention due to their ultimate atom utilization and great potential for highly cost-effective and high-efficiency HER electrocatalyst. Herein, we propose a high-temperature treatment strategy to furtherly improve the HER performance of atomically dispersed Pt-based catalyst. Interestingly, after appropriate high-temperature treatment on the atomically dispersed Pt0.8@CN, the Pt species on the designed N-doped porous carbon substrate with rich defect sites can be re-dispersed to single atom state with new coordination environment. The obtained Pt0.8@CN-1000 shows superior HER performance with overpotential of 13 mV at 10 mA cm−2 and mass activity of 11,284 mA/mgPt at −0.1 V, much higher than that of the pristine Pt0.8@CN and commercial Pt/C catalyst. The experimental and theoretical investigations indicate that the high-temperature treatment induces the restructuring of coordination environment and then the optimized Pt electronic state leads to the enhanced HER performances. This work affords new strategy and insights to develop the atomically dispersed high-efficiency catalysts.

CNTs were decorated onto Sr doped ZnO nanoparticles to construct an efficient photocatalyst via a facile sol-gel method. The as-fabricated Sr doped ZnO/CNTs with recyclability exhibits Sr and CNTs content dependent hydrogen evolution activit under visible light illumination. The Sr doped ZnO/CNTs photocatalyst shows the highest hydrogen evolution rate of 2732.2 μmolh−1g−1, which is 33.7 and 2.83 times higher than pure ZnO and Sr doped ZnO photocatalysts, respectively. The improved hydrogen evolution activity of Sr doped ZnO/CNTs is primarily assigned to high surface area, Sr doping and construction of heterojunction, which can extend the light absorption, decrease the optical band gap and improve the charge separation. Moreover, the underlying photocatalytic mechanism is proposed on the basis of Mott-Schottky study and explains the interfacial charge transfer process from ZnO to CNTs and Sr. This work open new strategies to synthesize CNTs based nanocomposite for hydrogen evolution.

Ni–Fe–Sn electrocatalyst supported on nickel foam (Ni–Fe–Sn/NF) with high efficiency of hydrogen evolution reaction (HER) has been successfully fabricated through one-step potentiostatic electrodeposition route. The optimized Ni–Fe–Sn/NF displayed an extremely low overpotential of, respectively, 144 and 180 mV at 50 and 100 mA cm−2 for HER in alkaline condition. Moreover, it could retain its superior stability for at least 12 h. The remarkable electrocatalytic activity of our electrocatalyst is ascribed to the high conductivity originated from synergistic effects between Ni, Fe, and Sn during HER process.

We investigated the hydrolysis of TiIV along with naturally abundant AlIII ions and reported the formation of a stable and semiconducting nanocluster. Interestingly, this compound exhibits an unusual odd-membered ring structure and also represents the largest Al-containing polyoxotitanium cluster (PTC) observed thus far. The presence of a shell of organic ligands as well as the incorporation of hetero-AlIII ions endowed the nanocluster with high air, thermal, and pH stabilities. The present compound exhibited a record photocatalytic hydrogen evolution of 402.88 μmol g−1 h−1 among PTC materials. This work not only paves the way towards stable PTC materials but also provides new insights into the design of novel photocatalysts.

Hydrogen is identified as the most promising zero-carbon fuel of the future. Naturally, in this regard, the hydrogen evolution reaction (HER), being a first critical step of the hydrogen technology and economy, attracts much attention. Conventionally, noble metals have been used as the electrocatalyst for HER, which in part holds back the hydrogen technology to become a large scale and heavily distributed energy technology. This has encouraged scientists to study cost-effective strategies for HER. Transition metal disulfides, being a low-cost material system with a great degree of engineering versatility, have recently emerged as a potential candidate that can significantly promote hydrogen evolution. Several studies have demonstrated that the control and manipulation of the structure and morphology of these materials can improve their proton reduction performance. This review covers many of the decisive factors and strategies to advance transition metal sulfides for HER applications.

Electrocatalytic N2 reduction provides an attractive alternative to Haber-Bosch process for artificial NH3 synthesis. The difficulty of suppressing competing proton reduction, however, largely impedes its practical use. Herein, we design a hydrophobic octadecanethiol-modified Fe3P nanoarrays supported on carbon paper (C18@Fe3P/CP) to effectively repel water, concentrate N2, and enhance N2-to-NH3 conversion. Such catalyst achieves an NH3 yield of 1.80 × 10−10 mol·s−1·cm−2 and a high Faradaic efficiency of 11.22% in 0.1 M Na2SO4, outperforming the non-modified Fe3P/CP (2.16 × 10−11 mol·s−1·cm−2, 0.9%) counterpart. Significantly, C18@Fe3P/CP renders steady N2-fixing activity/selectivity in cycling test and exhibits durability for at least 25 h. First-principles calculations suggest that the surface electronic structure and chemical activity of Fe3P can be well tuned by the thiol modification, which facilitates N2 electroreduction activity and catalytic formation of NH3.

In this study, with silicon carbide as a pyroelectric catalyst, the reactor was alternatively removed between a hot water bath and a cold water bath, which ensured the cold-hot circulation within 300–333 K at room temperature. Then the pyroelectric performance of silicon carbide was utilized in hydrogen evolution from water splitting. With methanol as the sacrificial agent, the hydrogen yield after 20 cycles was up to 32.84 μmol/g. Silicon carbide demonstrates high catalytic activity and together with its chemical stability, it shows potential in hydrogen production from water splitting under cold-hot alternation.

Catalytic performance of MoN, WN and WC on hydrogen evolution reaction (HER)were investigated by first-principles calculations, especially considering the effect of strain. From the calculation we can see the catalytic ability has an opposite trend with the adsorption capacity. H coverage was found to affect WN catalytic activity obviously, however has no effect on MoN and WC. Comparing with the experiments, we inferred that although the top site has the strongest potential catalytic ability, the actual catalytic site for HER is hollow1 site. Some specific transition metal doping (Ni > Fe > Mn > W for MoN, Fe > Co for WN, Ni > Co > Fe> Mn for WC) may indirectly improve the HER catalytic performance. It is worth noting that applying a certain strain (e.g. 2.5% tensile strain for MoN, 5% compressive strain for WN, WC) is helpful for improving the HER catalytic performance. Our work is instructive for HER catalyst development in terms of doping and strain.

Solar energy is an ideal energy source for solving energy shortages and serious environmental problems. In the past few decades, photocatalytic technology which uses solar energy to deal with the above problems has caused great interest. ZnIn2S4, as a layered ternary metal chalcogenide compound, has a series of advantages such as the wide light absorption range and adjustable bandgap. It has been applied in the different fields of photocatalysis in recent years. This review introduced the crystal structures and growth mechanism of ZnIn2S4 and summarized the preparation methods of ZnIn2S4. Also, the promoted strategies of ZnIn2S4 based photocatalytic system and their applications in the pollutant removal, hydrogen evolution, reduction of CO2, nitrogen fixation, and chemical synthesis was summarized. Furthermore, the challenges and development directions of the current ZnIn2S4 based photocatalytic system were proposed. It is hoped that this review will help researchers design a better ZnIn2S4 based photocatalytic system.

Researches on environmentally friendly semiconductor photocatalysts for efficient photocatalytic hydrogen evolution have important practical significance. Here, using first-principles calculations, the CeO2(111)/hBN heterojunction was conceived. The influence of the interface effect on the structural, electronic and optical properties of the heterojunction was investigated in detail. The band gap of the heterojunction is smaller than the two individual components and forms a type-II heterojunction, improving the photocatalytic activity. Furthermore, by doping two C atoms, the band gap of heterojunction was further narrowed. Both the oxidation and reduction potential of CeO2(111)/hBN heterojunction meet the requirements of water splitting and has certain advantages over other photocatalysts in the ability for photocatalytic hydrogen evolution. The study revealed the possible mechanism of CeO2(111) and hBN monolayers compositing to facilitate photocatalysis and hydrogen evolution ability, which may provide a possible reference direction for the practical design of more high-quality semiconductor photocatalysts.

Molybdenum disulfide (MoS2) is intrinsically inert for the hydrogen evolution reaction (HER) in alkaline media due to its electronic structures. Herein, we tune the electronic structures of MoS2 by a combined strategy of post-N doping coupled with the synergistic effect of Ti3C2TX. The as-prepared N-doped MoS2/Ti3C2TX heterostructures show remarkable alkaline HER activity with an overpotential of 225 mV at 140 mA cm-2, which ranks the N-doped MoS2/Ti3C2TX heterostructures among the best MoS2/MXene-based electrocatalysts reported for alkaline HER. The first-principles calculations indicate that the N doping can enhance the activation of nearby S sites of MoS2/Ti3C2TX and thus promote the HER process. This strategy provides a promising way to develop high-efficiency MoS2/MXene heterostructure catalysts for alkaline HER.

Electrocatalytic hydrogen evolution is an exercisable way to achieve large-scale application of hydrogen energy. It is of great significance to develop an effect, stable, and cost-effective electrocatalyst. Here, we applied the two-dimensional (2D) bismuth (Bi) to the electrocatalytic hydrogen evolution, and proposed the strategies to enhance the catalytic performance of the catalyst. Due to more active sites located along the edges of 2D structure, Bi nanosheets revealed a higher electrocatalytic activity (overpotential of −958 mV vs RHE at 10 mA cm−2, Tafel slope of 122 mV/dec) than the bulk counterpart. To further evaluate the electrocatalytic performance of Bi nanosheets, the typical parameters measured in different H+ concentration (C[H+]) are carried out. The improved catalytic activity obtained in 0.5 M H2SO4 is attributed to enhancing the hydrogen adsorption and accelerating the charge transport on the surface of catalyst. Moreover, the durability of Bi nanosheets has been texted, where the current is not evident fluctuation during the 40,000 s electrolysis measurement indicating its excellent stability. The present work expands the application of Bi in the catalysis and provides the simple strategies to improve its hydrogen evolution performance.

With the increasing concerns to energy shortage and environmental problems in modern society, the development of cheap, clean, and sustainable energy alternatives has been attracting tremendous attention globally. Among various strategies of renewable energy exploration, solar-driven water splitting into its compositional elements H2 and O2 is an ideal approach to convert and store renewable solar energy into chemical bonds. In recent few decades, as an emerging new type of catalysts, polyoxometalates (POMs) have been widely utilized for water splitting due to their versatile synthetic methodology and highly tunable physicochemical and photochemical properties. This critical review addresses the research advances of light-driven hydrogen evolution using polyoxometalate-based catalysts, including plenary POMs, transition-metal-substituted POMs, POM@MOF composites, and POM-semiconductor hybrids, under UV, near UV and visible light irradiation. In addition, the catalytic mechanism for each reaction system has been thoroughly discussed and summarized. Finally, a comprehensive outlook of this research area is also prospected.

A highly efficient, low-cost and environmentally friendly photocathode with long-term stability is the goal of practical solar hydrogen evolution applications. Here, we found that the Cu3BiS3 film-based photocathode meets the abovementioned requirements. The Cu3BiS3-based photocathode presents a remarkable onset potential over 0.9 VRHE with excellent photoelectrochemical current densities (~7 mA/cm2 under 0 VRHE) and appreciable 10-hour long-term stability in neutral water solutions. This high onset potential of the Cu3BiS3-based photocathode directly results in a good unbiased operating photocurrent of ~1.6 mA/cm2 assisted by the BiVO4 photoanode. A tandem device of Cu3BiS3-BiVO4 with an unbiased solar-to-hydrogen conversion efficiency of 2.04% is presented. This tandem device also presents high stability over 20 hours. Ultimately, a 5 × 5 cm2 large Cu3BiS3-BiVO4 tandem device module is fabricated for standalone overall solar water splitting with a long-term stability of 60 hours., A highly efficient, stable, low-cost and environmentally friendly photocathode is the goal of practical solar hydrogen evolution applications. Here, authors report a Cu3BiS3-based photocathode and Cu3BiS3-BiVO4 tandem cell for unbiased overall solar water splitting with a STH efficiency over 2%.

Two-dimensional (2D) metal oxides and chalcogenides (MOs & MCs) have been regarded as a new class of promising electro- and photocatalysts for many important chemical reactions such as hydrogen evolution reaction, CO2 reduction reaction and N2 reduction reaction in virtue of their outstanding physicochemical properties. However, pristine 2D MOs & MCs generally show the relatively poor catalytic performances due to the low electrical conductivity, few active sites and fast charge recombination. Therefore, considerable efforts have been devoted to engineering 2D MOs & MCs by rational structural design and chemical modification to further improve the catalytic activities. Herein, we comprehensively review the recent advances for engineering technologies of 2D MOs & MCs, which are mainly focused on the intercalation, doping, defects creation, facet design and compositing with functional materials. Meanwhile, the relationship between morphological, physicochemical, electronic, and optical properties of 2D MOs & MCs and their electro- and photocatalytic performances is also systematically discussed. Finally, we further give the prospect and challenge of the field and possible future research directions, aiming to inspire more research for achieving high-performance 2D MOs & MCs catalysts in energy storage and conversion fields.

Recently, carbon-based materials (e.g., graphene, carbon nanotubes, carbon quantum dots) have been used as electrocatalysts to catalyze the reactions such as hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR). Among them, graphene has attracted attention as an electrocatalyst, and its electrocatalytic performances have been improved by doping with metals and non-metals, surface and defect engineering, and hybrid development. In this perspective, the present paper reviewed the recent advances (2018 onwards) on the progress of graphene-based electrocatalysts for HER and overall water splitting (OWS). It is emphasizing strategies for optimizing electrocatalytic properties followed by challenges and future outlook. This review will provide the essential ideas and strategies that can help design graphene-based electrocatalysts of high performance that can be implemented for sustainable energy application.

The synthesis of NH-free pyrroles via Pd-catalyzed annulation of enaminones and alkenes is reported. With the catalysis of Pd(II), the activation of triple C(sp2)-H bonds, including one internal C(sp2)-H bond in enaminone, has been activated to provide various pyrroles. The interesting evolution of hydrogen gas from the reactions has been observed by a hydrogen detector.

Vacancy engineering is proposed to effectively modulate the hydrogen evolution reaction (HER) activity of M2CO2 MXene. A single C vacancy slightly weakens the H adsorption, while the introduction of a M vacancy or coupled M+C vacancies can greatly enhance the H binding. For a MXene with intrinsic too-strong H adsorption, double C vacancies are effective in weakening the binding and promoting the activity. The activity tuning is closely correlated to the electronic structures of the defected MXene, where the highest occupied peak position of the surface O electronic states shows an apparent linear trend with ΔGH and can be used to qualitatively predict the activity. The weakened or strengthened H adsorption by a C or M vacancy is attributed to the upshifted or downshifted Fermi level of surface O, respectively. Our results indicate the potential of defect chemistry to tune the catalytic activity of MXene and provide new possibilities to enhance the applications of MXene.

Photocatalytic hydrogen evolution from water has recently drawn tremendous attention and stimulated extensive efforts in the design of high-performance photocatalysts. Here, we designed a series of...

A hierarchical hollow tubular In2O3/ZnIn2S4 heterostructure was rationally designed by growing thin-layered ZnIn2S4 on the surface of carbon-coated hollow tubular In2O3 (C/HT-In2O3) that was derive...

Tuning the structural defects of graphite carbon nitride (g-C3N4) is an effective strategy to modify its band structure and promote charge separation, but it is still limited by complex and harsh p...

Hydrogen is a highly efficient and clean renewable energy source and water splitting through electrocatalytic hydrogen evolution is a most promising approach for hydrogen generation. Layered transition metal dichalcogenides-based nano-structures have recently attracted significant interest as robust and durable catalysts for hydrogen evolution. We systematically investigated the platinum (Pt) based dichalcogenides (PtS2, PtSe2 and PtTe2) as highly energetic and robust hydrogen evolution electrocatalysts. PtTe2 catalyst unveiled the rapid hydrogen evolution process with the low overpotentials of 75 and 92 mV (vs. RHE) at a current density of 10 mA cm−2, and the small Tafel slopes of 64 and 59 mV/dec in acidic and alkaline medium, respectively. The fabricated PtTe2 electrocatalyst explored a better catalytic activity than PtS2 and PtSe2. The density functional theory estimations explored that the observed small Gibbs free energy for H-adsorption of PtTe2 was given the prominent role to achieve the superior electrocatalytic and excellent stability activity towards hydrogen evolution due to a smaller bandgap and the metallic nature. We believe that this work will offer a key path to use Pt based dichalcogenides for hydrogen evolution electrocatalysts.

Hampered by the ambiguous mechanism of hydrogen evolution reaction (HER) in basic media, the exploration of highly efficient catalytically active sites for alkaline HER is of significance. Herein, a metal oxide Sr4Ru2O9 engineering a face-sharing [RuO6] octahedra motif was synthesized through the solid-state method, and served as HER electrocatalyst. Benefited from the Ru-Ru metallic bonding crossing the common plane, the H* adsorption and reaction energy barriers were optimized. Sr4Ru2O9 only required an ultra-small overpotential (ƞ10) of 28 mV at a current density of 10 mA cm−2 for HER in 1.0 M KOH with an exceptional stability (180 hours), outperforming the commercial Pt/C (ƞ10 = 38 mV). These findings suggest a fresh insight in designing novel active sites for electrocatalysis.

Delicate design and rapid development of low-cost, highly active, and perdurable pH-universal heterogenveous hydrogen evolution reaction (HER) electrocatalysts are demanding challenge in energy-conversion technologies. Herein, heterostructured CoP/MoO2 electrocatalyst was synthesized by employing MoO2 nanorods as framework for the growth of CoP nanoparticles. Owing to the fact that the effective interface of heterostructure can enhance electron transfer/mass diffusion and expose ample active sites, the CoP/MoO2 reveals eminent HER activities with favorable long-term stability in all pH electrolytes, overpotentials of 69, 78, and 165 mV in 0.5 M H2SO4, 1.0 M KOH, and 1.0 M PBS (phosphate-buffered solution) electrolytes were required for CoP/MoO2 to reach the current density of 10 mA cm−2. This work emphasizes that strategy of electronic structure engineering holds great promises in pH-universal HER electrocatalysts for energy storage and conversion.

g-C3N4 with π-delocalization was coordinated between urea and a small amount of 1,3,5-tris(4-aminophenyl)benzene (TAPB) (UCN-xTAPB) by a facile polymerization. Compared with pristine g-C3N4(UCN), t...

In this work, solar-heating-induced temperature-based photocatalytic hydrogen evolution reaction (PC-HER) of different photocatalysts (TiO2 P25, g-C3N4, and their loaded Pt) was comprehensively stu...

Redox non-innocent metal dithiolene or diamine complexes are potential alternative catalysts in hydrogen evolution reaction and have been incorporated into 2D metal–organic frameworks to obtain une...

The intrinsic activity of catalysts is crucial for the electrocatalytic hydrogen evolution reaction, which is essentially dependent on their crystal structure and surface electronic state. The vari...

Plasmon-mediated photocatalytic water splitting has attracted extensive attention due to its bright future in using visible light, but the enhancement mechanism is still unclear, and the efficiency...

To replace Pt-based compounds in the electrocatalytic hydrogen evolution reaction (HER), MoS2 has already been established as an efficient catalyst. The electrocatalytic activity of MoS2 is further...

An energy crisis is presently encountered with a promising opportunity for the rise of hydrogen technology, while feasible production of hydrogen calls for sophisticated structural design of water-...

Covalent functionalization has been demonstrated to be an effective strategy to improve the stability of monolayer black phosphorus (BP); however, the effect of chemical functionalization on the ca...

Urea electrolysis has prospects for urea-containing wastewater purification and hydrogen (H2) production, but the shortage of cost-effective catalysts restricts its development. In this work, the t...

Atomic layer deposition (ALD) of the iron-group transition-metal diselenides FeSe2, CoSe2, and NiSe2 is reported for the first time. The ALD processes employ the associated metal amidinates as the ...

The plasma semiconductor Cu2-xS has disclosed enormous potential in the field of broad-spectrum driven photocatalyst design due to its unique LSPR effect in the NIR region. Nevertheless, ineffective carrier separation and severe photocorrosion hinder the further functional applications of this promising material. Here, the TiO2@CuS double-shell nanoboxes were successfully constructed via a multistep control strategy involving template participation, and were firstly employed to broad-spectrum photocatalytic hydrogen evolution and pollutant elimination. The hollow core-shell nanocubes with LSPR effect have prominent advantages in broad-spectrum light response, improved photocharge separation and effective photocorrosion inhibition. Besides, the heterogeneous cavity structure also provides a larger specific surface area and ameliorates the light efficiency. Consequently, the optimized TiO2@CuS double-shell nanoboxes exhibit superior activity for H2 production under full-spectrum/NIR light irradiation (2467 and 173 μmol g−1 h−1, respectively), and maintain high activity in the photodegradation of stubborn pollutants. This work will motivate hollow photocatalysts designed to effectively utilize the spectrum and protect the sulfide core.

The limited stock of classical nonrenewable energy sources has motivated researchers to explore efficient strategies for sustainable and renewable energy production. Hydrogen production via electro...

Herein, first time we report that highly efficient sheet like leaf structure black TiO2 (LBT)/CdS hetero-structure (LBT/CdS). Photocatalytic hydrogen generation was tested for different material in the presence of visible light (λ ≥ 420 nm) irradiation. 10 wt% of LBT loaded CdS (10LBT/CdS) exhibit maximum photocatalytic H2 generation rate about ~10 mmol h−1 g−1, which is higher than the H2 production results of pristine CdS (6 mmol h−1 g−1) and leaf black-TiO2 5.1 mmol h−1 g−1) respectively. Detailed characterization revealed that higher photocatalytic activity was mainly attributed to enormous spatial transfer efficiency of photo-excited charge carriers at the hetero-junction between LBT and CdS in LBT/CdS. Additionally, introduction of 2D black leaf-TiO2 to CdS act as a mat and enhances the mobility of charge carriers. In addition, presence of anatase-rutile surface-phase junction in leaf TiO2 (synthesized at 750 °C) and more edges, steps and corners on the CdS synergistically increased the photocatalytic H2 generation and photocurrent response of LBT/CdS.

A designed type-II heterojunction photocatalyst, NiSe2/Cd0.5Zn0.5S (NiSe2/CZS), was successfully synthesized and it exhibits outstanding photocatalytic hydrogen evolution performance. The optimal loading amount of NiSe2 on Cd0.5Zn0.5S is 13 wt %, and the corresponding hydrogen production rate is approximately 121.01 mmol g−1 h−1 under visible light. The heterojunction structure between Cd0.5Zn0.5S and NiSe2 promoted the separation of photogenerated electron-hole pairs, effectively suppressed the photogenerated carrier recombination and endowed the material with excellent interfacial charge transfer properties, thus improving the photocatalytic performance.

Semiconductor-based photocatalytic hydrogen evolution is considered to be a promising and cost-effective approach to address the environmental issues and energy crisis. It still remains a great challenge to design highly-efficient semiconductor photocatalysts via a facile method. Herein, hierarchically porous hydrangea-like In2S3/In2O3 heterostructures are successfully synthesized via a simple in situ oxidization process. The formed In2S3/In2O3 heterostructures exhibit superior photocatalytic activity to the counterpart In2S3 and In2O3. The boosted photocatalytic performance is ascribed to the formed heterostructures, which greatly facilitate the interfacial charge transfer. Moreover, the formation of hierarchically porous heterostructures increases the number of active sites and improves the permeability, and thus significantly promotes the photocatalytic H2 evolution activity. This work may provide a new insight for designing In2S3-based heterostructures for efficient solar light conversion.

The growing energy concern all over the world has recognized hydrogen energy as the most promising renewable energy sources. Recently, electrocatalytic hydrogen evolution reaction (HER) by water splitting has been extensively studied with a focus on developing efficient electrocatalysts that can afford HER at overpotential with minimum power consumption. The two-dimensional transition metal carbides and nitride, also known as MXenes, are becoming the rising star in developing efficient electrocatalysts for HER, owing to their integrated chemical and electronic properties, e.g., metallic conductivity, variety of redox-active transition metals, high hydrophilicity, and tunable surface functionalities. In this review, the recent progress about the fundamental understanding and materials engineering of MXenes-based electrocatalysts is summarized in concern with two aspects: i) the regulation of the intrinsic properties of MXenes, which include the composition, surface functionality, and defects; and ii) MXenes-based composites for HER process. In the end, we summarize the present challenges concerning the efficiency of MXenes-based HER electrocatalysts and propose the directions of future research efforts.

In this study, four meso-expanded Co(III)corroles at meta-positions through Suzuki–Miyaura coupling reactions and their structural characterization are successfully accomplished and reported. An analysis of the structure–property relationships by spectroscopy, electrochemistry and electrochemical catalysis demonstrate how the positional isomerism influence the electronic structure and their catalytic behaviors of hydrogen evolution reactions (HERs) and oxygen reduction reactions (ORRs).

Hydrogen evolution from a weak acid, acetic acid, occurs at extremely high rates for iron tetraphenylporphyrin in the presence tertiary amine as a cocatalyst. Kinetic analysis of H2 evolution for a...