High-Performance H2 Photosynthesis from Pure Water over Ru-S Charge Transfer Channels.

As a versatile energy carrier, H2 is considered as one of the most promising sources of clean energy to tackle the current energy crisis and environmental concerns, which can be produced from photocatalytic water splitting. However, solar-driven photocatalytic H2 production from pure water in the absence of sacrificial reagents remains a great challenge. Herein, we demonstrate that the incorporation of Ru single atoms (SAs) into ZnIn2S4 (Ru-ZIS) can enhance the light absorption, reduce the energy barriers for water dissociation, and construct a channel (Ru-S) for separating photogenerated electron-hole pairs, as a result of a significantly enhanced photocatalytic water splitting process. Impressively, the productivity of H2 reaches 735.2 µmol g-1 h-1 under visible light irradiation in the absence of sacrificial agents. The apparent quantum efficiency (AQE) for H2 evolution reaches 7.5% at 420 nm, with a solar-to-hydrogen (STH) efficiency of 0.58%, which is much higher than the value of natural synthetic plants (∼0.10%). Moreover, Ru-ZIS exhibits steady productivity of H2 even after exposure to ambient conditions for 330 days. This work provides a unique strategy for constructing charge transfer channels to promote the separation of photogenerated electron-hole pairs, which may motivate the fundamental researches on catalyst design for photocatalysis and beyond.

Regulating the Electrochemical Nitrate Reduction Performance with Controllable Distribution of Unconventional Phase Copper on Alloy Nanostructures.

Electrochemical nitrate reduction reaction (NO3RR) is emerging as a promising strategy for nitrate removal and ammonia (NH3) production using renewable electricity. Although great progresses have been achieved, the crystal phase effect of electrocatalysts on NO3RR remains rarely explored. Here, the epitaxial growth of unconventional 2H Cu on hexagonal close-packed (hcp) IrNi template, resulting in the formation of three IrNiCu@Cu nanostructures, is reported. IrNiCu@Cu-20 shows superior catalytic performance, with NH3 Faradaic efficiency (FE) of 86% at -0.1 (vs reversible hydrogen electrode [RHE]) and NH3 yield rate of 687.3 mmol gCu -1 h-1, far better than common face-centered cubic Cu. In sharp contrast, IrNiCu@Cu-30 and IrNiCu@Cu-50 covered by hcp Cu shell display high selectivity toward nitrite (NO2 -), with NO2 - FE above 60% at 0.1 (vs RHE). Theoretical calculations have demonstrated that the IrNiCu@Cu-20 has the optimal electronic structures for NO3RR due to the highest d-band center and strongest reaction trend with the lowest energy barriers. The high electroactivity of IrNiCu@Cu-20 originates from the abundant low coordination of Cu sites on the surface, which guarantees the fast electron transfer to accelerate the intermediate conversions. This work provides a feasible tactic to regulate the product distribution of NO3RR by crystal phase engineering of electrocatalysts.

Metallic 1T/1T' phase TMD nanosheets with enhanced chemisorption sites for ultrahigh-efficiency lead removal.

Two-dimensional (2D) materials, as adsorbents, have garnered great attention in removing heavy metal ions (HMIs) from drinking water due to their extensive exposed adsorption sites. Nevertheless, there remains a paucity of experimental research to remarkably unlock their adsorption capabilities and fully elucidate their adsorption mechanisms. In this work, exceptional lead ion (Pb2+) (a common HMI) removal capacity (up to 758 mg g-1) is achieved using our synthesized metallic 1T/1T' phase 2D transition metal dichalcogenide (TMD, including MoS2, WS2, TaS2, and TiS2) nanosheets, which hold tremendous activated S chemisorption sites. The residual Pb2+ concentration can be reduced from 2 mg L-1 to 2 µg L-1 within 0.5 min, meeting the drinking water standards following World Health Organization guideline (Pb2+ concentrations <10 µg L-1). Atomic-scale characterizations and calculations based on density functional theory unveil that Pb2+ bond to the top positions of transition metal atoms in a single-atom form through the formation of S-Pb bonds. Point-of-use (POU) devices fabricated by our reported metallic phase MoS2 nanosheets exhibit treatment capacity of 55 L-water g-1-adsorbent for feed Pb2+ concentration of 1 mg L-1, which is 1-3 orders of magnitude higher than other 2D materials and commercial activated carbon.

Facet-Controlled Synthesis of Unconventional-Phase Metal Alloys for Highly Efficient Hydrogen Oxidation.

Facet control and phase engineering of metal nanomaterials are both important strategies to regulate their physicochemical properties and improve their applications. However, it is still a challenge to tune the exposed facets of metal nanomaterials with unconventional crystal phases, hindering the exploration of the facet effects on their properties and functions. In this work, by using Pd nanoparticles with unconventional hexagonal close-packed (hcp, 2H type) phase, referred to as 2H-Pd, as seeds, a selective epitaxial growth method is developed to tune the predominant growth directions of secondary materials on 2H-Pd, forming Pd@NiRh nanoplates (NPLs) and nanorods (NRs) with 2H phase, referred to as 2H-Pd@2H-NiRh NPLs and NRs, respectively. The 2H-Pd@2H-NiRh NRs expose more (100)h and (101)h facets on the 2H-NiRh shells compared to the 2H-Pd@2H-NiRh NPLs. Impressively, when used as electrocatalysts toward hydrogen oxidation reaction (HOR), the 2H-Pd@2H-NiRh NRs show superior activity compared to the NiRh alloy with conventional face-centered cubic (fcc) phase (fcc-NiRh) and the 2H-Pd@2H-NiRh NPLs, revealing the crucial role of facet control in enhancing the catalytic performance of unconventional-phase metal nanomaterials. Density functional theory (DFT) calculations further unravel that the excellent HOR activity of 2H-Pd@2H-NiRh NRs can be attributed to the more exposed (100)h and (101)h facets on the 2H-NiRh shells, which possess high electron transfer efficiency, optimized H* binding energy, enhanced OH* binding energy, and a low energy barrier for the rate-determining step during the HOR process.

Integrating Ozone Pollutant Elimination in N2 Electrolysis to Produce Nitrate with Reduced Reaction Steps.

The synthesis of nitrate by the electrochemical N2 oxidation reaction (NOR) is currently one of the most promising routes. However, the traditional generation of nitrate depends on the oxidation reaction between N2 and H2O (or ·OH), which involves complex reaction steps and intermediates, showing strong competition from oxygen evolution reaction (OER). Here, an effective NOR method is proposed to directly oxidize N2 by using O3 as a reactive oxygen source to reduce the reaction step. Electrochemical tests demonstrate that the nitrate yield of Pd-Mn3O4/CNT electrocatalyst reaches the milligram level, which is the highest yield reported so far for electrocatalytic NOR. Quantitative characterization is employed to establish a comprehensive set of benchmarks to confirm the intrinsic nature of nitrogen activation and test the O3-mediated reaction mechanism. Density functional theory (DFT) calculations show that the heterostructure Pd-Mn3O4 leads to a strong adsorption preference for N2 and O3, which greatly reduces the activation energy barrier for N2. This accelerates the synthesis of nitrate based on the direct formation mechanism, which reduces energy barriers and the reaction steps, thus increasing the performance of electrocatalytic nitrate production. The techno-economic analysis underscores the promising feasibility and sustainable economic value of the presented method.

Broadband Near-Infrared Light Excitation Generates Long-Lived Near-Infrared Luminescence in Gallates.

Persistent luminescence describes the phenomenon whereby luminescence remains after the stoppage of excitation. Recently, upconversion persistent luminescence (UCPL) phosphors that can be directly charged by near-infrared (NIR) light have gained considerable attention due to their promising applications ranging from photonics to biomedicine. However, current lanthanide-based UCPL phosphors show small absorption cross sections and low upconversion charging efficiency. The development of UCPL phosphors faces challenges due to the lack of flexible upconversion charging pathways and poor design flexibility. Herein, we discovered a lattice defect-mediated broadband photon upconversion process and the accompanying NIR-to-NIR UCPL in Cr-doped zinc gallate nanoparticles. The zinc gallate nanoparticles can be directly activated by broadband NIR light in the 700-1000 nm range to produce persistent luminescence at about 700 nm, which is also readily enhanced by rationally tailoring the lattice defects in the phosphors. This proposed UCPL phosphor achieved a signal-to-background ratio of over 200 in bioimaging by efficiently avoiding interference from autofluorescence and light scattering. Our work reported a lattice defect-mediated photon upconversion phenomenon, which significantly expands the horizons for the flexible design of UCPL phosphors toward broad applications ranging from bioimaging to photocatalysis.

Progress in Non-Fullerene Acceptors: Evolution from Small to Giant Molecules.

With the rapid development of non-fullerene acceptors (NFAs), the power conversion efficiency (PCE) of organic solar cells (OSCs) is increasing. According to their different chemical structures, NFAs can initially be divided into two categories: small molecule acceptors (SMAs) and polymerized small molecule acceptors (PSMAs). Due to the strong absorption capacity and controllable energy levels, the PCE of devices based on SMAs has approached 20%. Compared with SMAs, PSMAs have advantages in stability and flexibility, and the PCE of PSMA-based devices has exceeded 18%. However, the higher synthesis cost and lower batch repeatability hinder its further development. Recently, the concept of giant molecule acceptors (GMAs) has been proposed. These materials have a clear molecular structure and are considered novel acceptor materials that combine the advantages of SMAs and PSMAs. Currently, the PCE of devices based on GMAs has exceeded 19%. In this review, we will introduce the latest developments in SMAs, PSMAs, and GMAs. Then, the advantages of GMAs and the relationship between their structure and performance will be analyzed. In the end, perspectives on the opportunities and challenges of these materials are provided, which could inspire further development of NFAs for advanced OSCs.

How liquids charge the superhydrophobic surfaces.

Liquid-solid contact electrification (CE) is essential to diverse applications. Exploiting its full implementation requires an in-depth understanding and fine-grained control of charge carriers (electrons and/or ions) during CE. Here, we decouple the electrons and ions during liquid-solid CE by designing binary superhydrophobic surfaces that eliminate liquid and ion residues on the surfaces and simultaneously enable us to regulate surface properties, namely work function, to control electron transfers. We find the existence of a linear relationship between the work function of superhydrophobic surfaces and the as-generated charges in liquids, implying that liquid-solid CE arises from electron transfer due to the work function difference between two contacting surfaces. We also rule out the possibility of ion transfer during CE occurring on superhydrophobic surfaces by proving the absence of ions on superhydrophobic surfaces after contact with ion-enriched acidic, alkaline, and salt liquids. Our findings stand in contrast to existing liquid-solid CE studies, and the new insights learned offer the potential to explore more applications.

Tuning Vertical Electrodeposition for Dendrites-Free Zinc-Ion Batteries.

Manipulating the crystallographic orientation of zinc deposition is recognized as an effective approach to address zinc dendrites and side reactions for aqueous zinc-ion batteries (ZIBs). We introduce 2-methylimidazole (Mlz) additive in zinc sulfate (ZSO) electrolyte to achieve vertical electrodeposition with preferential orientation of the (100) and (110) crystal planes. Significantly, the zinc anode exhibited long lifespan with 1500 h endurance at 1 mA cm-2 and an excellent 400 h capability at a depth of discharge (DOD) of 34% in Zn||Zn battery configurations, while in Zn||MnO2 battery assemblies, a capacity retention of 68.8% over 800 cycles is attained. Theoretical calculation reveals that the strong interactions between Mlz and (002) plane impeding its growth, while Zn atoms exhibit lower migration energy barrier and superior mobility on (100) and (110) crystal planes guaranteed the heightened mobility of zinc atoms on the (100) and (110) crystal planes, thus ensuring their superior ZIB performance than that with only ZSO electrolyte, which offers a route for designing next-generation high energy density ZIB devices.

Selective Oxidation of sp-Bonded Carbon in Graphdiyne/Carbon Nanotubes Heterostructures to Form Dominant Epoxy Groups for Two-Electron Oxygen Reduction.

Two-electron oxygen reduction reaction (2e- ORR) is of great significance to H2O2 production and reversible nonalkaline Zn-air batteries (ZABs). Multiple oxygen-containing sp2-bonded nanocarbons have been developed as electrocatalysts for 2e- ORR, but they still suffer from poor activity and stability due to the limited and mixed active sites at the edges as well as hydrophilic character. Herein, graphdiyne (GDY) with rich sp-C bonds is studied for enhanced 2e- ORR. First, computational studies show that GDY has a favorable formation energy for producing five-membered epoxy ring-dominated groups, which is selective toward the 2e- ORR pathway. Then based on the difference in chemical activity of sp-C bonds in GDY and sp2-C bonds in CNTs, we experimentally achieved conductive and hydrophobic carbon nanotubes (CNTs) covering O-modified GDY (CNTs/GDY-O) through a mild oxidation treatment combined with an in situ CNTs growth approach. Consequently, the CNTs/GDY-O exhibits an average Faraday efficiency of 91.8% toward H2O2 production and record stability over 330 h in neutral media. As a cathode electrocatalyst, it greatly extends the lifetime of 2e- nonalkaline ZABs at both room and subzero temperatures.

Site-Selective Growth of fcc-2H-fcc Copper on Unconventional Phase Metal Nanomaterials for Highly Efficient Tandem CO2 Electroreduction.

Copper (Cu) nanomaterials are a unique kind of electrocatalysts for high-value multi-carbon production in carbon dioxide reduction reaction (CO2RR), which holds enormous potential in attaining carbon neutrality. However, phase engineering of Cu nanomaterials remains challenging, especially for the construction of unconventional phase Cu-based asymmetric heteronanostructures. Here the site-selective growth of Cu on unusual phase gold (Au) nanorods, obtaining three kinds of heterophase fcc-2H-fcc Au-Cu heteronanostructures is reported. Significantly, the resultant fcc-2H-fcc Au-Cu Janus nanostructures (JNSs) break the symmetric growth mode of Cu on Au. In electrocatalytic CO2RR, the fcc-2H-fcc Au-Cu JNSs exhibit excellent performance in both H-type and flow cells, with Faradaic efficiencies of 55.5% and 84.3% for ethylene and multi-carbon products, respectively. In situ characterizations and theoretical calculations reveal the co-exposure of 2H-Au and 2H-Cu domains in Au-Cu JNSs diversifies the CO* adsorption configurations and promotes the CO* spillover and subsequent C-C coupling toward ethylene generation with reduced energy barriers.

Dynamic multicolor emissions of multimodal phosphors by Mn2+ trace doping in self-activated CaGa4O7.

The manipulation of excitation modes and resultant emission colors in luminescent materials holds pivotal importance for encrypting information in anti-counterfeiting applications. Despite considerable achievements in multimodal and multicolor luminescent materials, existing options generally suffer from static monocolor emission under fixed external stimulation, rendering them vulnerability to replication. Achieving dynamic multimodal luminescence within a single material presents a promising yet challenging solution. Here, we report the development of a phosphor exhibiting dynamic multicolor photoluminescence (PL) and photo-thermo-mechanically responsive multimodal emissions through the incorporation of trace Mn2+ ions into a self-activated CaGa4O7 host. The resulting phosphor offers adjustable emission-color changing rates, controllable via re-excitation intervals and photoexcitation powers. Additionally, it demonstrates temperature-induced color reversal and anti-thermal-quenched emission, alongside reproducible elastic mechanoluminescence (ML) characterized by high mechanical durability. Theoretical calculations elucidate electron transfer pathways dominated by intrinsic interstitial defects and vacancies for dynamic multicolor emission. Mn2+ dopants serve a dual role in stabilizing nearby defects and introducing additional defect levels, enabling flexible multi-responsive luminescence. This developed phosphor facilitates evolutionary color/pattern displays in both temporal and spatial dimensions using readily available tools, offering significant promise for dynamic anticounterfeiting displays and multimode sensing applications.

Controlled Synthesis of Unconventional Phase Alloy Nanobranches for Highly Selective Electrocatalytic Nitrite Reduction to Ammonia.

The controlled synthesis of metal nanomaterials with unconventional phases is of significant importance to develop high-performance catalysts for various applications. However, it remains challenging to modulate the atomic arrangements of metal nanomaterials, especially the alloy nanostructures that involve different metals with distinct redox potentials. Here we report the general one-pot synthesis of IrNi, IrRhNi and IrFeNi alloy nanobranches with unconventional hexagonal close-packed (hcp) phase. Notably, the as-synthesized hcp IrNi nanobranches demonstrate excellent catalytic performance towards electrochemical nitrite reduction reaction (NO2RR), with superior NH3 Faradaic efficiency and yield rate of 98.2 % and 34.6 mg h-1 mgcat -1 (75.5 mg h-1 mgIr -1) at 0 and -0.1 V (vs reversible hydrogen electrode), respectively. Ex/in situ characterizations and theoretical calculations reveal that the Ir-Ni interactions within hcp IrNi alloy improve electron transfer to benefit both nitrite activation and active hydrogen generation, leading to a stronger reaction trend of NO2RR by greatly reducing energy barriers of rate-determining step.

Self-Powered and Self-Recoverable Multimodal Force Sensors Based on Trap State and Interfacial Electron Transfer.

Multi-dimensional force sensing that combines intensity, location, area and the like could gather a wealth of information from mechanical stimuli. Developing materials with force-induced optical and electrical dual responses would provide unique opportunities to multi-dimensional force sensing, with electrical signals quantifying the force amplitude and the luminescence output providing spatial distribution of force. However, the reliance on external power supply and high-energy excitation source brings significant challenges to the applicability of multi-dimensional force sensors. Here we reported the mechanical energy-driven and sunlight-activated materials with force-induced dual responses, and investigated the underlying mechanisms of self-sustainable force sensing. Theoretical analysis and experimental data unraveled that trap-controlled luminescence and interfacial electron transfer play a major role in force-induced optical and electrical output. These materials were manufactured into pressure sensor with renewable dual-mode output for quantifying and visualization of pressures by electrical and optical output, respectively, without power supply and high-energy irradiation. The quantification of tactile sensation and stimuli localization of mice highlighted the multi-dimensional sensing ability of the sensor. Overall, this self-powered pressure sensor with multimodal output provides more modalities of force sensing, poised to change the way that intelligent devices sense with the world.

Pt-Modified High Entropy Rare Earth Oxide for Efficient Hydrogen Evolution in pH-Universal Environments.

The development of efficient and stable catalysts for hydrogen production from electrolytic water in a wide pH range is of great significance in alleviating the energy crisis. Herein, Pt nanoparticles (NPs) anchored on the vacancy of high entropy rare earth oxides (HEREOs) were prepared for the first time for highly efficient hydrogen production by water electrolysis. The prepared Pt-(LaCeSmYErGdYb)O showed excellent electrochemical performances, which require only 12, 57, and 77 mV to achieve a current density of 100 mA cm-2 in 0.5 M H2SO4, 1.0 M KOH, and 1.0 M PBS environments, respectively. In addition, Pt-(LaCeSmYErGdYb)O has successfully worked at 400 mA cm-2 @ 60 °C for 100 h in 0.5 M H2SO4, presenting the high mass activity of 37.7 A mg-1Pt and turnover frequency (TOF) value of 38.2 s-1 @ 12 mV, which is far superior to the recently reported hydrogen evolution reaction (HER) catalysts. Density functional theory (DFT) calculations have revealed that the interactions between Pt and HEREO have optimized the electronic structures for electron transfer and the binding strength of intermediates. This further leads to optimized proton binding and water dissociation, supporting the highly efficient and robust HER performances in different environments. This work provides a new idea for the design of efficient RE-based electrocatalysts.

Dilute Aqueous-Aprotic Electrolyte Towards Robust Zn-Ion Hybrid Supercapacitor with High Operation Voltage and Long Lifespan.

With the merits of the high energy density of batteries and power density of supercapacitors, the aqueous Zn-ion hybrid supercapacitors emerge as a promising candidate for applications where both rapid energy delivery and moderate energy storage are required. However, the narrow electrochemical window of aqueous electrolytes induces severe side reactions on the Zn metal anode and shortens its lifespan. It also limits the operation voltage and energy density of the Zn-ion hybrid supercapacitors. Using 'water in salt' electrolytes can effectively broaden their electrochemical windows, but this is at the expense of high cost, low ionic conductivity, and narrow temperature compatibility, compromising the electrochemical performance of the Zn-ion hybrid supercapacitors. Thus, designing a new electrolyte to balance these factors towards high-performance Zn-ion hybrid supercapacitors is urgent and necessary. We developed a dilute water/acetonitrile electrolyte (0.5 m Zn(CF3SO3)2 + 1 m LiTFSI-H2O/AN) for Zn-ion hybrid supercapacitors, which simultaneously exhibited expanded electrochemical window, decent ionic conductivity, and broad temperature compatibility. In this electrolyte, the hydration shells and hydrogen bonds are significantly modulated by the acetonitrile and TFSI- anions. As a result, a Zn-ion hybrid supercapacitor with such an electrolyte demonstrates a high operating voltage up to 2.2 V and long lifespan beyond 120,000 cycles.

Highly Active CoNi-CoN3 Composite Sites Synergistically Accelerate Oxygen Electrode Reactions in Rechargeable Zinc-Air Batteries.

Reaching rapid reaction kinetics of oxygen reduction (ORR) and oxygen evolution reactions (OER) is critical for realizing efficient rechargeable zinc-air batteries (ZABs). Herein, a novel CoNi-CoN3 composite site containing CoNi alloyed nanoparticles and CoN3 moieties is first constructed in N-doped carbon nanosheet matrix (CoNi-CoN3/C). Benefiting from the high electroactivity of CoNi-CoN3 composite sites and large surface area, CoNi-CoN3/C shows a superior half-wave potential (0.88 V versus RHE) for ORR and a small overpotential (360 mV) for OER at 10 mA cm-2. Theoretical calculations have demonstrated that the introduction of CoNi alloys has modulated the electronic distributions near the CoN3 moiety, inducing the d-band center of CoNi-CoN3 composite site to shift down, thus stabilizing the valence state of Co active sites and balancing the adsorption of OER/ORR intermediates. Accordingly, the reaction energy trends exhibit optimized overpotentials for OER/ORR, leading to superior battery performances. For aqueous and flexible quasi-solid-state rechargeable ZABs with CoNi-CoN3/C as catalyst, a large power density (250 mW cm-2) and high specific capacity (804 mAh g-1) are achieved. The in-depth understanding of the electroactivity enhancement mechanism of interactive metal nanoparticles and metal coordinated with nitrogen (MNx) moieties is crucial for designing novel high-performance metal/nitrogen-doped carbon (M─N─C) catalysts.

Implanting oxophilic metal in PtRu nanowires for hydrogen oxidation catalysis.

Bimetallic PtRu are promising electrocatalysts for hydrogen oxidation reaction in anion exchange membrane fuel cell, where the activity and stability are still unsatisfying. Here, PtRu nanowires were implanted with a series of oxophilic metal atoms (named as i-M-PR), significantly enhancing alkaline hydrogen oxidation reaction (HOR) activity and stability. With the dual doping of In and Zn atoms, the i-ZnIn-PR/C shows mass activity of 10.2 A mgPt+Ru-1 at 50 mV, largely surpassing that of commercial Pt/C (0.27 A mgPt-1) and PtRu/C (1.24 A mgPt+Ru-1). More importantly, the peak power density and specific power density are as high as 1.84 W cm-2 and 18.4 W mgPt+Ru-1 with a low loading (0.1 mg cm-2) anion exchange membrane fuel cell. Advanced experimental characterizations and theoretical calculations collectively suggest that dual doping with In and Zn atoms optimizes the binding strengths of intermediates and promotes CO oxidation, enhancing the HOR performances. This work deepens the understanding of developing novel alloy catalysts, which will attract immediate interest in materials, chemistry, energy and beyond.

Coordination Environment Engineering of Metal Centers in Coordination Polymers for Selective Carbon Dioxide Electroreduction toward Multicarbon Products.

Electrocatalytic carbon dioxide reduction reaction (CO2RR) toward value-added chemicals/fuels has offered a sustainable strategy to achieve a carbon-neutral energy cycle. However, it remains a great challenge to controllably and precisely regulate the coordination environment of active sites in catalysts for efficient generation of targeted products, especially the multicarbon (C2+) products. Herein we report the coordination environment engineering of metal centers in coordination polymers for efficient electroreduction of CO2 to C2+ products under neutral conditions. Significantly, the Cu coordination polymer with Cu-N2S2 coordination configuration (Cu-N-S) demonstrates superior Faradaic efficiencies of 61.2% and 82.2% for ethylene and C2+ products, respectively, compared to the selective formic acid generation on an analogous polymer with the Cu-I2S2 coordination mode (Cu-I-S). In situ studies reveal the balanced formation of atop and bridge *CO intermediates on Cu-N-S, promoting C-C coupling for C2+ production. Theoretical calculations suggest that coordination environment engineering can induce electronic modulations in Cu active sites, where the d-band center of Cu is upshifted in Cu-N-S with stronger selectivity to the C2+ products. Consequently, Cu-N-S displays a stronger reaction trend toward the generation of C2+ products, while Cu-I-S favors the formation of formic acid due to the suppression of C-C couplings for C2+ pathways with large energy barriers.

In Situ Reconstruction of High-Entropy Heterostructure Catalysts for Stable Oxygen Evolution Electrocatalysis under Industrial Conditions.

Despite of urgent needs for highly stable and efficient electrochemical water-splitting devices, it remains extremely challenging to acquire highly stable oxygen evolution reaction (OER) electrocatalysts under harsh industrial conditions. Here, a successful in situ synthesis of FeCoNiMnCr high-entropy alloy (HEA) and high-entropy oxide (HEO) heterocatalysts via a Cr-induced spontaneous reconstruction strategy is reported, and it is demonstrated that they deliver excellent ultrastable OER electrocatalytic performance with a low overpotential of 320 mV at 500 mA cm-2 and a negligible activity loss after maintaining at 100 mA cm-2 for 240 h. Remarkably, the heterocatalyst holds outstanding long-term stability under harsh industrial condition of 6 m KOH and 85 °C at a current density of as high as 500 mA cm-2 over 500 h. Density functional theory calculations reveal that the formation of the HEA-HEO heterostructure can provide electroactive sites possessing robust valence states to guarantee long-term stable OER process, leading to the enhancement of electroactivity. The findings of such highly stable OER heterocatalysts under industrial conditions offer a new perspective for designing and constructing efficient high-entropy electrocatalysts for practical industrial water splitting.