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Photocatalytic performance can be optimized via introduction of reactive sites. However, it is practically difficult to engineer these on specific photocatalyst surfaces, because of limited understanding of atomic‐level structure‐activity. Here we report a facile sonication‐assisted chemical reduction for specific facets regulation via oxygen deprivation on Bi‐based photocatalysts. The modified Bi2MoO6 nanosheets exhibit 61.5 and 12.4 μmol g−1 for CO and CH4 production respectively, ≈3 times greater than for pristine catalyst, together with excellent stability/reproducibility of ≈20 h. By combining advanced characterizations and simulation, we confirm the reaction mechanism on surface‐regulated photocatalysts, namely, induced defects on highly‐active surface accelerate charge separation/transfer and lower the energy barrier for surface CO2 adsorption/activation/reduction. Promisingly, this method appears generalizable to a wider range of materials. [ABSTRACT FROM AUTHOR]

Potassium‐ion batteries hold practical potential for large‐scale energy storage owing to their appealing cell voltage and cost‐effective features. The development of anode materials with high rate capability and satisfactory cycle lifespan, however, is one of the key elements for exploiting this electrochemical energy storage system at practical levels. Here, a template‐assisted strategy is reported for acquiring a bimetallic telluride heterostructure which is supported on N‐doped carbon shell (ZnTe/CoTe2@NC) that promotes diffusion of K+ ions for rapid charge transfer. It is shown that in telluride heterojunctions, electron‐rich Te sites and built‐in electric fields contributed by electron transfer from ZnTe to CoTe2 concomitantly provide abundant cation adsorption sites and facilitate interfacial electron transport during potassiation/depotassiation. The relatively fine ZnTe/CoTe2 nanoparticles imparted by the heterojunction result in high structural stability, together with a highly reversible capacity up to 5000 cycles at 5 A g−1. Moreover, using judiciously combined experiment and theoretical computation, it is demonstrated that the energy barrier for K+ diffusion in telluride heterojunctions is significantly lower than that in individual counterparts. This quantitative design for fast and durable charge transfer in telluride heterostructures can be of immediate benefit for the rational design of batteries for low‐cost energy storage and conversion. [ABSTRACT FROM AUTHOR]

Electroreduction of carbon dioxide (CO2) into multicarbon products provides possibility of large-scale chemicals production and is therefore of significant research and commercial interest. However, the production efficiency for ethanol (EtOH), a significant chemical feedstock, is impractically low because of limited selectivity, especially under high current operation. Here we report a new silver–modified copper–oxide catalyst (dCu2O/Ag2.3%) that exhibits a significant Faradaic efficiency of 40.8% and energy efficiency of 22.3% for boosted EtOH production. Importantly, it achieves CO2–to–ethanol conversion under high current operation with partial current density of 326.4 mA cm−2 at −0.87 V vs reversible hydrogen electrode to rank highly significantly amongst reported Cu–based catalysts. Based on in situ spectra studies we show that significantly boosted production results from tailored introduction of Ag to optimize the coordinated number and oxide state of surface Cu sites, in which the *CO adsorption is steered as both atop and bridge configuration to trigger asymmetric C–C coupling for stablization of EtOH intermediates. It is of high interest to convert CO2 into valuable ethanol product. Here the authors demonstrate the asymmetric C-C coupling triggered on Ag-modified oxide-derived Cu sites can accelerate and steer the reaction pathway for ethanol production with high faradaic efficiency and current density. [ABSTRACT FROM AUTHOR]

Metal sulfides electrodeposition in sulfur cathodes mitigates the shuttle effect of polysulfides to achieve high Coulombic efficiency in secondary metal-sulfur batteries. However, fundamental understanding of metal sulfides electrodeposition and kinetics mechanism remains limited. Here using room-temperature sodium-sulfur cells as a model system, we report a Mo5N6 cathode material that enables efficient Na2S electrodeposition to achieve an initial discharge capacity of 512 mAh g−1 at a specific current of 1 675 mA g−1, and a final discharge capacity of 186 mAh g−1 after 10,000 cycles. Combined analyses from synchrotron-based spectroscopic characterizations, electrochemical kinetics measurements and density functional theory computations confirm that the high d-band position results in a low Na2S2 dissociation free energy for Mo5N6. This promotes Na2S electrodeposition, and thereby favours long-term cell cycling performance. Incomplete conversion of sodium polysulfides represents a significant issue in room-temperature sodium-sulfur batteries. Here, the authors propose Mo5N6 as an electrocatalyst for efficient Na2S electrodeposition and improved cell cycling performances. [ABSTRACT FROM AUTHOR]

Understanding the late stages of the electrochemical CO2 reduction reaction (CRR) in the formation of various C2 products provides great opportunities for fully achieving a selective CRR to target products. Here, we report, for the first time, that C2 product (including ethylene, ethane and ethanol) selectivity can be directed by the active site's oxygen affinity on a range of non-metal doped copper surfaces (Cu–X). Through theoretical evaluation of adsorption energetics of key post-C2-coupling intermediates, we demonstrate how branching reaction pathways are competing with each other and how selectivity for different products is achieved. The oxygen affinities of different active sites on Cu–X catalysts, including the dopant atom and Cu sites, are identified as descriptors for C2 product selectivity. The ethylene pathway is shown to be favored on Cu–X surfaces doped with strong oxygen affinity atoms, such as boron. Ethane selectivity is generally boosted by Cu–X, whereas ethanol generation is suppressed by non-metal doping on Cu surfaces. Bader charge analyses of electron distribution on intermediates and electronegativity analyses of non-metal dopant atoms are integrated to identify the impact of intrinsic electronic properties on adsorption behaviour, together with the resultant C2 product selectivity on Cu–X catalysts. Our findings shed light on controlling product selectivity by modulating oxygen affinity in complex electrochemical reactions. [ABSTRACT FROM AUTHOR]