Abstract Oxygen reduction reaction towards hydrogen peroxide (H 2 O ) provides a green alternative route for H production, but it lacks efficient catalysts to achieve high selectivity and activity simultaneously under industrial-relevant production rates. Here we report boron-doped carbon (B-C) catalyst which can overcome this activity-selectivity dilemma. Compared the state-of-the-art oxidized catalyst, B-C presents enhanced (saving more than 210 mV overpotential) currents (up 300 mA cm −2...

Oxygen reduction reaction (ORR) is one of the most important electrochemical reactions. Starting from a common intermediate *-O-OH, ORR splits into two pathways, either producing hydrogen peroxide (H

A single nickel atom embedded in graphene is one of the most representative single-atom catalysts, and it has a high activity selectivity for electrochemical CO2 reduction (CO2R) to CO. However, catalytic origin, especially coordination structure Ni, remains highly puzzling, as previous density functional theory (DFT) calculations showed that all possible structures should be inactive and/or nonselective. Here, using ab initio molecular dynamics (AIMD) "slow-growth" sampling approach...

Electrochemical oxygen reduction to hydrogen peroxide (H2O2) in acidic media, especially proton exchange membrane (PEM) electrode assembly reactors, suffers from low selectivity and the lack of low-cost catalysts. Here we present a cation-regulated interfacial engineering approach promote H2O2 (over 80%) under industrial-relevant generation rates 400 mA cm-2) strong media using just carbon black catalyst small number alkali metal cations, representing 25-fold improvement compared that...

The long-term stability of single-atom catalysts is a major factor affecting their large-scale commercial application. How to evaluate the dynamic under working conditions still lacking. Here, taking single copper atom embedded in N-doped graphene as an example, "constant-potential hybrid-solvation model" used reversible transformation between atoms and clusters realistic reaction conditions. It revealed that adsorption H vital driving force for leaching Cu from catalyst surface. more...

Direct methanol fuel cells (DMFCs) are promising power sources for portable electronic devices. Atomically dispersed M–N–C cathode catalysts demonstrated a great potential in addressing the high-cost and crossover issues DMFCs.

Electrochemical water oxidation reaction (WOR) to hydrogen peroxide (H2O2) via a 2e- pathway provides sustainable H2O2 synthetic route, but is challenged by the traditional 4e- counterpart of oxygen evolution. Here we report CO2/carbonate mediation approach steering WOR from 2e-. Using fluorine-doped tin oxide electrode in carbonate solutions, achieved high selectivity up 87%, and delivered unprecedented partial currents 1.3 A cm-2, which represents orders magnitude improvement compared...

Abstract Electrolytes play a critical role in stabilizing highly reactive lithium‐metal anodes (LMAs) and high‐voltage cathodes for rechargeable batteries (LMBs). Localized high concentration electrolytes (LHCEs) have achieved remarkable success the context of LMBs. However, state‐of‐the‐art LHCEs are based on LiFSI salt, which is prohibitively expensive. Here, utility low‐cost LiPF 6 salt localized saturated (LSEs) with series solvents diluents LMBs cobalt‐free LiNiO 2 cathode...

Oxygen reduction reaction (ORR) is essential to various renewable energy technologies. An important catalyst for ORR single iron atoms embedded in nitrogen-doped graphene (Fe-N-C). However, the rate-limiting step of on Fe-N-C unknown, significantly impeding understanding and improvement. Here, we report activation energies all steps, calculated by ab initio molecular dynamics simulations under constant electrode potential. In contrast common belief that a hydrogenation limits rate, find...

Selective electrochemical two-electron oxygen reduction is a promising route for renewable and on-site H2O2 generation as an alternative to the anthraquinone process. Herein, we report high-performance nitrogen-coordinated single-atom Pd electrocatalyst, which derived from Pd-doped zeolitic imidazolate frameworks (ZIFs) through one-step thermolysis. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) combined with X-ray absorption spectroscopy verifies...

Abstract Efficient CO 2 separation technologies are essential for mitigating climate change. Compared to traditional thermochemical methods, electrochemically mediated carbon capture using redox-tunable sorbents emerges as a promising alternative due its versatility and energy efficiency. However, the undesirable linear free-energy relationship between redox potential binding affinity in existing chemistry makes it fundamentally challenging optimise key sorbent properties independently via...

Improving the selectivity of electrochemical CO

Abstract Perovskite light‐emitting diodes (LEDs) require small grain sizes to spatially confine charge carriers for efficient radiative recombination. As size decreases, passivation of surface defects becomes increasingly important. Additionally, polycrystalline perovskite films are highly brittle and mechanically fragile, limiting their practical applications in flexible electronics. In this work, the introduction properly chosen bulky organo‐ammonium halide additives is shown be able...

3DOM MoSe₂@C constructed by ultrathin MoSe₂ nanosheets strongly binging on carbon skeleton exerts high energy and power density for sodium-ion batteries.

Abstract The coupling of the carbon dioxide reduction reaction (CO 2 RR) and methanol oxidation (MOR) holds great promise for energy‐efficient production HCOO − . However, anode catalysts' limited selectivity (<80%) stability (<15 h) have impeded electron utilization rates. To overcome it, copper‐copper(I) oxide‐copper(II) oxide nanowires (Cu─CuO─Cu O NWs) catalysts been developed, which exhibit exceptional performance in promoting MOR with a faradic efficiency nearly 100% at...

Cube-shaped nanocrystals (NCs) of conventional metals like gold and silver generally exhibit localized surface plasmon resonance (LSPR) in the visible region with spectral modes determined by their faceted shapes. However, NCs exhibiting LSPR response infrared (IR) are relatively rare. Here, we describe colloidal synthesis nanoscale fluorine-doped indium oxide (F:In2O3) cubes IR region, wherein fluorine was found to both direct cubic morphology act as an aliovalent dopant. Single-crystalline...

Selenium and tellurium in Li–S batteries: formation of polyselenosulfides enables improved sulfur redox kinetics while polytellurosulfides improves lithium cycling efficiency.

The interaction of water with the CaO(001) surface has been studied from ultrahigh-vacuum to submillibar vapor pressures and at temperatures 100 300 K using well-structured CaO(001)/Mo(001) thin-film model systems. Infrared reflection absorption spectroscopy (IRAS), X-ray photoelectron (XPS), scanning tunneling microscopy (STM) in combination density functional theory (DFT) calculations have employed reveal correlation between vibrational frequencies hydroxyl groups distinct hydroxylated...

Abstract Hydrazine‐assisted water electrolyzer is a promising energy‐efficient alternative to conventional electrolyzer, offering an appealing path for sustainable hydrogen (H 2 ) production with reduced energy consumption. However, such presently impeded by lacking efficient catalyst accelerate the kinetics of pivotal half‐reaction, that is, hydrazine oxidation reaction (HzOR). Herein, ruthenium (Ru) single‐atom on octahedral cobalt oxide (Co 3 O 4 substrate (Ru‐Co catalyst, guided...

Spin-polarized density functional theory calculations have been performed to investigate the mechanisms for CxHy formation on Fe3C(100). It is found that H-assisted CO dissociation (CO + H → CHO; CHO CH O) has lower barrier than direct C O), but surface Cs atom hydrogenation form CsH most favored pathway. As first C2 species, ketenylidene CsCO rising from adsorption an important intermediate C2Hx formation. Initial forms instead of dissociation. The CsCH, CsHCH and CsH2CH close effective...

Formation of partly dissociated water chains is observed on CaO(001) films upon exposure at 300 K. While morphology and orientation the 1D assemblies are revealed from scanning tunneling microscopy, their atomic structure identified with infrared absorption spectroscopy combined density functional theory calculations. The latter exploit an ab initio genetic algorithm linked to atomistic thermodynamics determine low-energy H2O configurations oxide surface. development structures C4v symmetric...

The shifts of core-level binding energies can provide powerful information about the electronic structure a material. Understanding physical origin these for catalytically relevant oxides may important insight into their properties. This requires reliable theoretical methods which are able to relate energy structure. In order establish such methodology, CaO(100) surface bulk have been studied with Hartree-Fock and density-functional theory using both cluster periodic slab models. obtained...