Showing papers on "Overpotential published in 2021"

Modulating electronic structure of metal-organic frameworks by introducing atomically dispersed Ru for efficient hydrogen evolution.

Abstract: Developing high-performance electrocatalysts toward hydrogen evolution reaction is important for clean and sustainable hydrogen energy, yet still challenging. Herein, we report a single-atom strategy to construct excellent metal-organic frameworks (MOFs) hydrogen evolution reaction electrocatalyst (NiRu0.13-BDC) by introducing atomically dispersed Ru. Significantly, the obtained NiRu0.13-BDC exhibits outstanding hydrogen evolution activity in all pH, especially with a low overpotential of 36 mV at a current density of 10 mA cm−2 in 1 M phosphate buffered saline solution, which is comparable to commercial Pt/C. X-ray absorption fine structures and the density functional theory calculations reveal that introducing Ru single-atom can modulate electronic structure of metal center in the MOF, leading to the optimization of binding strength for H2O and H*, and the enhancement of HER performance. This work establishes single-atom strategy as an efficient approach to modulate electronic structure of MOFs for catalyst design. Developing high-performance, neutral-media H2-evolution electrocatalysts is important for clean and sustainable hydrogen energy, yet rare, expensive elements are most active. Here, authors show that metal-organic frameworks modified with single ruthenium atoms as high-performances catalysts.

Engineering single-atomic ruthenium catalytic sites on defective nickel-iron layered double hydroxide for overall water splitting.

Abstract: Rational design of single atom catalyst is critical for efficient sustainable energy conversion. However, the atomic-level control of active sites is essential for electrocatalytic materials in alkaline electrolyte. Moreover, well-defined surface structures lead to in-depth understanding of catalytic mechanisms. Herein, we report a single-atomic-site ruthenium stabilized on defective nickel-iron layered double hydroxide nanosheets (Ru1/D-NiFe LDH). Under precise regulation of local coordination environments of catalytically active sites and the existence of the defects, Ru1/D-NiFe LDH delivers an ultralow overpotential of 18 mV at 10 mA cm−2 for hydrogen evolution reaction, surpassing the commercial Pt/C catalyst. Density functional theory calculations reveal that Ru1/D-NiFe LDH optimizes the adsorption energies of intermediates for hydrogen evolution reaction and promotes the O–O coupling at a Ru–O active site for oxygen evolution reaction. The Ru1/D-NiFe LDH as an ideal model reveals superior water splitting performance with potential for the development of promising water-alkali electrocatalysts. Rational design of single atom catalyst is critical for efficient sustainable energy conversion. Single-atomic-site ruthenium stabilized on defective nickel-iron layered double hydroxide nanosheets achieve superior HER and OER performance in alkaline media.

Platinum single-atom catalyst coupled with transition metal/metal oxide heterostructure for accelerating alkaline hydrogen evolution reaction.

Abstract: Single-atom catalysts provide an effective approach to reduce the amount of precious metals meanwhile maintain their catalytic activity. However, the sluggish activity of the catalysts for alkaline water dissociation has hampered advances in highly efficient hydrogen production. Herein, we develop a single-atom platinum immobilized NiO/Ni heterostructure (PtSA-NiO/Ni) as an alkaline hydrogen evolution catalyst. It is found that Pt single atom coupled with NiO/Ni heterostructure enables the tunable binding abilities of hydroxyl ions (OH*) and hydrogen (H*), which efficiently tailors the water dissociation energy and promotes the H* conversion for accelerating alkaline hydrogen evolution reaction. A further enhancement is achieved by constructing PtSA-NiO/Ni nanosheets on Ag nanowires to form a hierarchical three-dimensional morphology. Consequently, the fabricated PtSA-NiO/Ni catalyst displays high alkaline hydrogen evolution performances with a quite high mass activity of 20.6 A mg−1 for Pt at the overpotential of 100 mV, significantly outperforming the reported catalysts. While H2 evolution from water may represent a renewable energy source, there is a strong need to improve catalytic efficiencies while maximizing materials utilization. Here, authors examine single-atom Pt on nickel-based heterostructures as highly active electrocatalysts for alkaline H2 evolution.

Single Atom Ruthenium-Doped CoP/CDs Nanosheets via Splicing of Carbon-Dots for Robust Hydrogen Production

Abstract: Ultrathin two-dimensional catalysts are attracting attention in the field of electrocatalytic hydrogen evolution. This work describe a composite material design in which CoP nanoparticles doped with Ru single-atom sites supported on carbon dots (CDs) single-layer nanosheets formed by splicing CDs (Ru CoP/CDs). Small CD fragments bore abundant functional groups, analogous to pieces of a jigsaw puzzle, and could provide a high density of binding sites to immobilize Ru CoP. The single-particle-thick nanosheets formed by splicing CDs acted as supports, which improved the conductivity of the electrocatalyst and the stability of the catalyst during operation. The Ru CoP/CDs formed from doping atomic Ru dispersed on CoP showed very high efficiency for the hydrogen evolution reaction (HER) over a wide pH range. The catalyst prepared under optimized conditions displayed outstanding stability and activity: the overpotential for the HER at a current density of 10 mA cm was as low as 51 and 49 mV under alkaline and acidic conditions, respectively. Density functional theory calculations showed that the substituted Ru single atoms lowered the proton-coupled electron transfer energy barrier and promoted H−H bond formation, thereby enhancing catalytic performance for the HER. The findings open a new avenue for developing carbon-based hybridization materials with integrated electrocatalytic performance for water splitting. 1 1 1 −2

Pt Single Atoms Supported on N-Doped Mesoporous Hollow Carbon Spheres with Enhanced Electrocatalytic H 2 -Evolution Activity

Abstract: The electronic metal-support interaction (EMSI) plays a crucial role in catalysis as it can induce electron transfer between metal and support, modulate the electronic state of the supported metal, and optimize the reduction of intermediate species In this work, the tailoring of electronic structure of Pt single atoms supported on N-doped mesoporous hollow carbon spheres (Pt1 /NMHCS) via strong EMSI engineering is reported The Pt1 /NMHCS composite is much more active and stable than the nanoparticle (PtNP ) counterpart and commercial 20 wt% Pt/C for catalyzing the electrocatalytic hydrogen evolution reaction (HER), exhibiting a low overpotential of 40 mV at a current density of 10 mA cm-2 , a high mass activity of 207 A mg-1 Pt at 50 mV overpotential, a large turnover frequency of 2018 s-1 at 300 mV overpotential, and outstanding durability in acidic electrolyte Detailed spectroscopic characterizations and theoretical simulations reveal that the strong EMSI effect in a unique N1 -Pt1 -C2 coordination structure significantly tailors the electronic structure of Pt 5d states, resulting in promoted reduction of adsorbed proton, facilitated H-H coupling, and thus Pt-like HER activity This work provides a constructive route for precisely designing single-Pt-atom-based robust electrocatalysts with high HER activity and durability

Sodium-Decorated Amorphous/Crystalline RuO2 with Rich Oxygen Vacancies: A Robust pH-Universal Oxygen Evolution Electrocatalyst

Abstract: The oxygen evolution reaction (OER) is a key reaction for many electrochemical devices. To date, many OER electrocatalysts function well in alkaline media, but exhibit poor performances in neutral and acidic media, especially the acidic stability. Herein, sodium-decorated amorphous/crystalline RuO 2 with rich oxygen vacancies (a/c-RuO 2 ) was developed as a pH-universal OER electrocatalyst. The a/c-RuO 2 shows remarkable resistance to acid corrosion and oxidation during OER, which leads to an extremely high catalytic stability, as confirmed by a negligible overpotential increase after continuously catalyzing OER for 60 h at pH = 1. Besides, a/c-RuO 2 also exhibits superior OER activities to commercial RuO 2 and most reported OER catalysts under all pH conditions. Theoretical calculations indicated that the introduction of Na dopant and oxygen vacancy in RuO 2 weakens the adsorption strength of the OER intermediates by engineering the d -band center, thereby lowering the energy barrier for OER.

Nickel ferrocyanide as a high-performance urea oxidation electrocatalyst

Abstract: Urea is often present in waste water but can be used in powering fuel cells and as an alternative oxidation substrate to water in an electrolyser. However, an insufficient mechanistic understanding and the lack of efficient catalysts for the urea oxidation reaction have hampered the development of such applications. Here we demonstrate that a nickel ferrocyanide (Ni2Fe(CN)6) catalyst supported on Ni foam can drive the urea oxidation reaction with a higher activity and better stability than those of conventional Ni-based catalysts. Our experimental and computational data suggest a urea oxidation reaction pathway different from most other Ni-based catalysts that comprise NiOOH derivatives as the catalytically active compound. Ni2Fe(CN)6 appears to be able to directly facilitate a two-stage reaction pathway that involves an intermediate ammonia production (on the Ni site) and its decomposition to N2 (on the Fe site). Owing to the different rate-determining steps with more favourable thermal/kinetic energetics, Ni2Fe(CN)6 achieves a 100 mA cm−2 anodic current density at a potential of 1.35 V (equal to an overpotential of 0.98 V). Urea oxidation could be a lower-energy alternative to water oxidation in hydrogen-producing electrolysers, but improved catalysts are required to facilitate the reaction. Geng et al. report nickel ferrocyanide as a promising catalyst and suggest that it operates via a different pathway to that of previous materials.

Stable and Highly Efficient Hydrogen Evolution from Seawater Enabled by an Unsaturated Nickel Surface Nitride

Abstract: Electrocatalytic production of hydrogen from seawater provides a route to low-cost and clean energy conversion. However, the hydrogen evolution reaction (HER) using seawater is greatly hindered by the lack of active and stable catalysts. Herein, an unsaturated nickel surface nitride (Ni-SN@C) catalyst that is active and stable for the HER in alkaline seawater is prepared. It achieves a low overpotential of 23 mV at a current density of 10 mA cm-2 in alkaline seawater electrolyte, which is superior to Pt/C. Compared to conventional transition metal nitrides or metal/metal nitride heterostructures, the Ni-SN@C has no detectable bulk nickel nitride phase. Instead, unsaturated NiN bonding on the surface is present. In situ Raman measurements show that the Ni-SN@C performs like Pt with the ability to generate hydronium ions in a high-pH electrolyte. The catalyst operation is then demonstrated in a two-electrode electrolyzer system, coupling with hydrazine oxidation at the anode. Using this system, a cell voltage of only 0.7 V is required to achieve a current density of 1 A cm-2 .

High‐Entropy Metal Sulfide Nanoparticles Promise High‐Performance Oxygen Evolution Reaction

Abstract: Transition metal sulfides with a multi‐elemental nature represent a class of promising catalysts for oxygen evolution reaction (OER) owing to their good catalytic activity. However, their synthesis remains a challenge due to the thermodynamic immiscibility of the constituent multimetallic elements in a sulfide structure. Herein, for the first time the synthesis of high‐entropy metal sulfide (HEMS, i.e., (CrMnFeCoNi)Sx) solid solution nanoparticles is reported. Computational and X‐ray photoelectron spectroscopy analysis suggest that the (CrMnFeCoNi)Sx exhibits a synergistic effect among metal atoms that leads to desired electronic states to enhance OER activity. The (CrMnFeCoNi)Sx nanoparticles show one of the best activities (low overpotential 295 mV at 100 mA cm−2 in 1 m KOH solution) and good durability (only slight polarization after 10 h by chronopotentiometry) compared with their unary, binary, ternary, and quaternary sulfide counterparts. This work opens up a new synthesis paradigm for high‐entropy compound nanoparticles for highly efficient electrocatalysis applications.

Vertically-interlaced NiFeP/MXene electrocatalyst with tunable electronic structure for high-efficiency oxygen evolution reaction

Abstract: Layered double hydroxides (LDHs) with decent oxygen evolution reaction (OER) activity have been extensively studied in the fields of energy storage and conversion. However, their poor conductivity, ease of agglomeration, and low intrinsic activity limit their practical application. To date, improvement of the intrinsic activity and stability of NiFe-LDHs through the introduction of heteroatoms or its combination with other conductive substrates to enhance their water-splitting performance has drawn increasing attention. In this study, vertically interlaced ternary phosphatised nickel/iron hybrids grown on the surface of titanium carbide flakes (NiFeP/MXene) were successfully synthesised through a hydrothermal reaction and phosphating calcination process. The optimised NiFeP/MXene exhibited a low overpotential of 286 mV at 10 mA cm−2 and a Tafel slope of 35 mV dec−1 for the OER, which exceeded the performance of several existing NiFe-based catalysts. NiFeP/MXene was further used as a water-splitting anode in an alkaline electrolyte, exhibiting a cell voltage of only 1.61 V to achieve a current density of 10 mA cm−2. Density functional theory (DFT) calculations revealed that the combination of MXene acting as a conductive substrate and the phosphating process can effectively tune the electronic structure and density of the electrocatalyst surface to promote the energy level of the d-band centre, resulting in an enhanced OER performance. This study provides a valuable guideline for designing high-performance MXene-supported NiFe-based OER catalysts.

Trimetallic Spinel NiCo2-xFexO4 Nanoboxes for Highly Efficient Electrocatalytic Oxygen Evolution.

Abstract: The development of efficient and low-cost electrocatalysts toward the oxygen evolution reaction (OER) is critical for improving the efficiency of several electrochemical energy conversion and storage devices. Here, we report an elaborate design and synthesis of porous Co-based trimetallic spinel oxide nanoboxes (NiCo2-x Fex O4 NBs) by a novel metal-organic framework engaged strategy, which involves chemical etching, cation exchange, and subsequent thermal oxidation processes. Owing to the structural and compositional advantages, the optimized trimetallic NiCo2-x Fex O4 NBs (x is about 0.117) deliver superior electrocatalytic performance for OER with an overpotential of 274 mV at 10 mA cm-2 , a small Tafel slope of 42 mV dec-1 , and good stability in alkaline electrolyte, which is much better than that of Co-based bi/monometallic spinel oxides and even commercial RuO2 .

A NiCo LDH nanosheet array on graphite felt: an efficient 3D electrocatalyst for the oxygen evolution reaction in alkaline media

Abstract: The development of efficient electrocatalysts from Earth-abundant elements for the oxygen evolution reaction (OER) is highly desired. Here, we report the electrodeposition of a NiCo layered double hydroxide nanosheet array on graphite felt (NiCo LDHs/GF) as a 3D OER electrocatalyst. Such NiCo LDHs/GF exhibits superior electrocatalytic activity with the need for an overpotential of 249 mV to drive a current density of 20 mA cm−2 in 1.0 M KOH. It also shows strong long-term electrochemical durability with its activity being maintained for at least 24 h.

Fluorination-enabled Reconstruction of NiFe Electrocatalysts for Efficient Water Oxidation.

Abstract: Developing low-cost and efficient electrocatalysts to accelerate oxygen evolution reaction (OER) kinetics is vital for water and carbon-dioxide electrolyzers. The fastest-known water oxidation catalyst, Ni(Fe)OxHy, usually produced through an electrochemical reconstruction of precatalysts under alkaline condition, has received substantial attention. However, the reconstruction in the reported catalysts usually leads to a limited active layer and poorly controlled Fe-activated sites. Here, we demonstrate a new electrochemistry-driven F-enabled surface-reconstruction strategy for converting the ultrathin NiFeOxFy nanosheets into an Fe-enriched Ni(Fe)OxHy phase. The activated electrocatalyst shows a low OER overpotential of 218 ± 5 mV at 10 mA cm-2 and a low Tafel slope of 31 ± 4 mV dec-1, which is among the best for NiFe-based OER electrocatalysts. Such superior performance is caused by the effective formation of the Fe-enriched Ni(Fe)OxHy active-phase that is identified by operando Raman spectroscopy and the substantially improved surface wettability and gas-bubble-releasing behavior.

High-valent bimetal Ni3S2/Co3S4 induced by Cu doping for bifunctional electrocatalytic water splitting

Abstract: Rational design of low-cost and efficient electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is imperative for renewable energy conversion. Herein, for the first time, a facile strategy is developed to synthesize M (M = Fe, Cu, Zn, Mo) doped bimetallic sulfide heterostructure Ni3S2/Co3S4 electrocatalysts. The as-prepared bifunctional Cu-Ni3S2/Co3S4 electrode exhibits excellent electrocatalytic activity for HER and OER in 1 M KOH electrolyte, and it requires only an overpotential of 79 mV (150 mV) to deliver 10 mA cm−2 (20 mA cm-2) current density for HER process. Moreover, it shows a considerable low cell voltage of 1.49 V at the current density of 10 mA cm-2 in a two-electrode configuration which is far surpassing most of the reported bifunctional metal sulfides. Meanwhile, besides increasing the specific surface area of the electrocatalyst by optimizing the microstructure, the introduction of Cu cation could also stimulate the formation of high-valent Ni/Co sites, which can be verified by XPS technique. Density function theory calculations demonstrate that the Cu-doping boosts the formation of high valent Co sites and enhances the charge transfer performance of Ni and Co species, thus promotes intrinsic catalytic activity through modulating the d-band center of Co and reducing the adsorption energy of H and O-containing intermediates (H*, OH*, OOH*) on the surface of the catalyst. This work suggests the importance of exploitation of transition metal ion-doping for promoting the electrocatalytic activity of bimetallic sulfides.

Recent advances in highly active nanostructured NiFe LDH catalyst for electrochemical water splitting

Abstract: Highly efficient, low-cost electrocatalysts having superior activity and stability are crucial for practical electrochemical water splitting, which involves hydrogen and oxygen evolution reactions (HER and OER). The sustainable production of hydrogen fuel from electrochemical water splitting requires the development of a highly efficient and stable electrocatalyst with low overpotential that drives electrochemical redox reactions. Electrochemical water splitting using highly active nickel-iron layered double hydroxide (NiFe LDH) catalyst having a very high turnover frequency and mass activity is considered as a potential contender in the area of electrocatalysis owing to the practical challenges including high efficiency and long durability at low overpotential, which shows great potential in future hydrogen economy. This review includes certain recommendations on enhancing the electrocatalytic performance of NiFe LDH-based electrocatalyst, particularly through morphology engineering, construction of hierarchical/core–shell nanostructures, and doping of heteroatoms through combined experimental assessment and theoretical investigations, which in turn improve the electrocatalytic performance. Finally, emphasis is made on the bifunctional activity of the NiFe LDH catalyst for overall water splitting. At the end, the conclusions and future outlook for the design of the NiFe LDH catalyst towards scale-up for their use as electrolyzer at the industrial level are also discussed.

Role of the Carbon-Based Gas Diffusion Layer on Flooding in a Gas Diffusion Electrode Cell for Electrochemical CO 2 Reduction

Abstract: The deployment of gas diffusion electrodes (GDEs) for the electrochemical CO2 reduction reaction (CO2RR) has enabled current densities an order of magnitude greater than those of aqueous H cells. The gains in production, however, have come with stability challenges due to rapid flooding of GDEs, which frustrate both laboratory experiments and scale-up prospects. Here, we investigate the role of carbon gas diffusion layers (GDLs) in the advent of flooding during CO2RR, finding that applied potential plays a central role in the observed instabilities. Electrochemical characterization of carbon GDLs with and without catalysts suggests that the high overpotential required during electrochemical CO2RR initiates hydrogen evolution on the carbon GDL support. These potentials impact the wetting characteristics of the hydrophobic GDL, resulting in flooding that is independent of CO2RR. Findings from this work can be extended to any electrochemical reduction reaction using carbon-based GDEs (CORR or N2RR) with cathodic overpotentials of less than -0.65 V versus a reversible hydrogen electrode.

A Glass-Ceramic with Accelerated Surface Reconstruction toward the Efficient Oxygen Evolution Reaction.

Abstract: The effective non-precious metal catalysts toward the oxygen evolution reaction (OER) are highly desirable for electrochemical water splitting. Herein, we prepare a novel glass-ceramic (Ni1.5 Sn@triMPO4 ) by embedding crystalline Ni1.5 Sn nanoparticles into amorphous trimetallic phosphate (triMPO4 ) matrix. This unique crystalline-amorphous nanostructure synergistically accelerates the surface reconstruction to active Ni(Fe)OOH, due to the low vacancy formation energy of Sn in glass-ceramic and high adsorption energy of PO43- at the VO sites. Compared to the control samples, this dual-phase glass-ceramic exhibits a remarkably lowered overpotential and boosted OER kinetics after surface reconstruction, rivaling most of state-of-the-art electrocatalysts. The residual PO43- and intrinsic VO sites induce redistribution of electron states, thus optimizing the adsorption of OH* and OOH* intermediates on metal oxyhydroxides and promoting the OER activity.

Phosphorus Induced Electron Localization of Single Iron Sites for Boosted CO2 Electroreduction Reaction

Abstract: Electrochemical reduction of carbon dioxide (CO 2 ) into chemicals and fuels has recently attracted much interest, but normally suffers from a high overpotential and low selectivity. In this work, single P atoms were introduced into a N-doped carbon supported single Fe atom catalyst (Fe- SAC /NPC) mainly in the form of P-C bonds for CO 2 electroreduction to CO in an aqueous solution. This catalyst exhibited a CO Faradaic efficiency of ~97% at a low overpotential of 320 mV, and a Tafel slope of only 59 mV dec -1 , comparable to state-of-the-art gold catalysts. Experimental analysis combined with DFT calculations suggested that single P atom in high coordination shells (n ≥ 3), in particular the third coordination shell of Fe center enhanced the electronic localization of Fe, which improved the stabilization of the key *COOH intermediate on Fe, leading to superior CO 2 electrochemical reduction performance at low overpotentials.

Oxygen-evolving catalytic atoms on metal carbides.

Abstract: Single-atom catalysts have shown promising performance in various catalytic reactions. Catalytic metal sites supported on oxides or carbonaceous materials are usually strongly coordinated by oxygen or heteroatoms, which naturally affects their electronic environment and consequently their catalytic activity. Here, we reveal the stabilization of single-atom catalysts on tungsten carbides without the aid of heteroatom coordination for efficient catalysis of the oxygen evolution reaction (OER). Benefiting from the unique structure of tungsten carbides, the atomic FeNi catalytic sites are weakly bonded with the surface W and C atoms. The reported catalyst shows a low overpotential of 237 mV at 10 mA cm−2, which can even be lowered to 211 mV when the FeNi content is increased, a high turnover frequency value of 4.96 s−1 (η = 300 mV) and good stability (1,000 h). Density functional theory calculations show that either metallic Fe/Ni atoms or (hydro)oxide FeNi species are responsible for the high OER activity. We suggest that the application of inexpensive and durable WCx supports opens up a promising pathway to develop further single-atom catalysts for electrochemical catalytic reactions Metal oxides or carbonaceous supported atomic metal sites coordinated by oxygen or heteroatoms exhibit enhanced electrocatalytic activity. Stabilization of single-atom catalysts on tungsten carbides without heteroatom coordination for efficient oxygen evolution reaction is demonstrated.

Graphene/MoS2/FeCoNi(OH)x and Graphene/MoS2/FeCoNiPx multilayer-stacked vertical nanosheets on carbon fibers for highly efficient overall water splitting

Abstract: Development of excellent and cheap electrocatalysts for water electrolysis is of great significance for application of hydrogen energy. Here, we show a highly efficient and stable oxygen evolution reaction (OER) catalyst with multilayer-stacked hybrid structure, in which vertical graphene nanosheets (VGSs), MoS2 nanosheets, and layered FeCoNi hydroxides (FeCoNi(OH)x) are successively grown on carbon fibers (CF/VGSs/MoS2/FeCoNi(OH)x). The catalyst exhibits excellent OER performance with a low overpotential of 225 and 241 mV to attain 500 and 1000 mA cm−2 and small Tafel slope of 29.2 mV dec−1. Theoretical calculation indicates that compositing of FeCoNi(OH)x with MoS2 could generate favorable electronic structure and decrease the OER overpotential, promoting the electrocatalytic activity. An alkaline water electrolyzer is established using CF/VGSs/MoS2/FeCoNi(OH)x anode for overall water splitting, which generates a current density of 100 mA cm−2 at 1.59 V with excellent stability over 100 h. Our highly efficient catalysts have great prospect for water electrolysis. While water-splitting electrocatalysis offers a renewable means for carbon-neutral energy production, it is a challenge to design efficient, active, and stable catalysts. Here, authors prepare multilayer composite nanosheet materials as bifunctional water-splitting electrocatalysts.

Highly active and selective oxygen reduction to H2O2 on boron-doped carbon for high production rates

Abstract: Oxygen reduction reaction towards hydrogen peroxide (H2O2) provides a green alternative route for H2O2 production, but it lacks efficient catalysts to achieve high selectivity and activity simultaneously under industrial-relevant production rates. Here we report a boron-doped carbon (B-C) catalyst which can overcome this activity-selectivity dilemma. Compared to the state-of-the-art oxidized carbon catalyst, B-C catalyst presents enhanced activity (saving more than 210 mV overpotential) under industrial-relevant currents (up to 300 mA cm−2) while maintaining high H2O2 selectivity (85–90%). Density-functional theory calculations reveal that the boron dopant site is responsible for high H2O2 activity and selectivity due to low thermodynamic and kinetic barriers. Employed in our porous solid electrolyte reactor, the B-C catalyst demonstrates a direct and continuous generation of pure H2O2 solutions with high selectivity (up to 95%) and high H2O2 partial currents (up to ~400 mA cm−2), illustrating the catalyst’s great potential for practical applications in the future. Oxygen reduction reaction provides an environmentally-benign route for hydrogen peroxide production but lacks efficient catalysts to achieve high selectivity and activity simultaneously. Here, the authors report a boron-doped carbon catalyst which shows great promise with outstanding performance.

Rational strain engineering of single-atom ruthenium on nanoporous MoS2 for highly efficient hydrogen evolution.

Abstract: Maximizing the catalytic activity of single-atom catalysts is vital for the application of single-atom catalysts in industrial water-alkali electrolyzers, yet the modulation of the catalytic properties of single-atom catalysts remains challenging. Here, we construct strain-tunable sulphur vacancies around single-atom Ru sites for accelerating the alkaline hydrogen evolution reaction of single-atom Ru sites based on a nanoporous MoS2-based Ru single-atom catalyst. By altering the strain of this system, the synergistic effect between sulphur vacancies and Ru sites is amplified, thus changing the catalytic behavior of active sites, namely, the increased reactant density in strained sulphur vacancies and the accelerated hydrogen evolution reaction process on Ru sites. The resulting catalyst delivers an overpotential of 30 mV at a current density of 10 mA cm−2, a Tafel slope of 31 mV dec−1, and a long catalytic lifetime. This work provides an effective strategy to improve the activities of single-atom modified transition metal dichalcogenides catalysts by precise strain engineering. The modulation of single-atom catalyst properties for industrial applications remains challenging. Here, authors use strain engineering to amplify the synergistic effect between MoS2’s sulphur vacancies and single-atom Ru sites and accelerate H2 evolution electrocatalysis.

A hierarchical CuO@NiCo layered double hydroxide core–shell nanoarray as an efficient electrocatalyst for the oxygen evolution reaction

Abstract: Developing hierarchical electrocatalysts for the oxygen evolution reaction (OER) is of great importance for electrochemical hydrogen production. Here, we describe the development of a hierarchical CuO@NiCo layered double hydroxide core–shell nanoarray on copper foil (CuO@NiCo LDH/CF) as a 3D OER electrocatalyst. When tested in 1.0 M KOH, such CuO@NiCo LDH/CF offers superior catalytic activity with a geometrical catalytic current density of 20 mA cm−2 at an overpotential of only 256 mV. It also shows strong long-term electrochemical durability to retain its activity for at least 24 h.

Ni2P/NiMoP heterostructure as a bifunctional electrocatalyst for energy-saving hydrogen production

Abstract: Electrochemical water splitting is a sustainable and feasible strategy for hydrogen production but is hampered by the sluggish anodic oxygen evolution reaction (OER). Herein, an effective approach is introduced to significantly decrease the cell voltage by replacing the anodic OER with a urea oxidation reaction (UOR). A Ni2P/NiMoP nanosheet catalyst with a hierarchical architecture is uniformly grown on a nickel foam (NF) substrate through a simple hydrothermal and phosphorization method. The Ni2P/NiMoP achieves impressive HER activity, with a low overpotential of only 22 mV at 10 mA cm–2 and a low Tafel slope of 34.5 mV dec–1. In addition, the oxidation voltage is significantly reduced from 1.49 V to 1.33 V after the introduction of 0.33 M urea. Notably, a two-electrode electrolyzer employing Ni2P/NiMoP as a bifunctional catalyst exhibits a current density of 10 mA cm–2 at a cell voltage of 1.35 V and excellent long-term durability after 80 h.

In-situ construction of lattice-matching NiP2/NiSe2 heterointerfaces with electron redistribution for boosting overall water splitting

Abstract: High-efficiency electrocatalysts for water splitting can be achieved by constructing heterostructure engineering purposely. The same pyrite structure of NiSe2/NiP2 with admirable electrical conductivity of NiSe2 and outstanding stability of NiP2 is designed to boost electrocatalytic performance towards overall water splitting. Density functional theory (DFT) calculations identify that constructing NiP2/NiSe2 heterointerfaces with good lattice matching and the redistribution of electron between the heterointerfacecan optimize adsorption/desorption energy of H* effectively. Therefore, NiP2/NiSe2 heterostructure on carbon fiber cloth with one-step phosphoselenization is developed as electrocatalysts. As expected, NiP2/NiSe2 exhibits excellent catalytic activity with only 160 mV overpotential to realize a current density of 100 mA cm−2 and exceptional stability over 90 h at the current density of 10 mA cm−2 for HER in alkaline solution. This heterostructure strategy might be a new break-through for modulating the single-phase transition metal and designing highly active and durable catalysts towards water splitting.