The grain boundary in copper-based electrocatalysts has been demonstrated to improve the selectivity of solar-driven electrochemical CO2 reduction toward multicarbon products. However, approach form boundaries copper is still limited. This paper describes a controllable growth electrodeposition via poly(vinylpyrrolidone) used as an additive. A grain-boundary-rich metallic could be obtained convert into ethylene and ethanol with high 70% over wide potential range. In situ attenuated total...

Abstract The active sites for CO 2 electroreduction (CO R) to multi-carbon (C 2+ ) products over oxide-derived copper (OD-Cu) catalysts are under long-term intense debate. This paper describes the atomic structure motifs product-specific on OD-Cu in R. Herein, we describe realistic surface models by simulating process via molecular dynamic simulation with neural network (NN) potential. After analysis of 150 through NN potential based high-throughput testing, coupled density functional theory...

Abstract Artificial photosynthesis can be used to store solar energy and reduce CO 2 into fuels potentially alleviate global warming the crisis. Compared generation of gaseous products, it remains a great challenge tune product distribution artificial liquid fuels, such as CH 3 OH, which are suitable for storage transport. Herein, we describe introduction metallic Cu nanoparticles (NPs) on O films change from products bare predominantly OH by reduction in aqueous solutions. The specifically...

Abstract It is of great significance to reveal the detailed mechanism neighboring effects between monomers, as they could not only affect intermediate bonding but also change reaction pathway. This paper describes electronic effect Zn/Co monomers effectively promoting CO 2 electroreduction CO. Zn and Co atoms coordinated on N doped carbon (ZnCoNC) show a faradaic efficiency 93.2 % at −0.5 V versus RHE during 30‐hours test. Extended X‐ray absorption fine structure measurements (EXAFS)...

Tuning the facet exposure of Cu could promote multi-carbon (C2+) products formation in electrocatalytic CO2 reduction. Here we report design and realization a dynamic deposition-etch-bombardment method for Cu(100) facets control without using capping agents polymer binders. The synthesized Cu(100)-rich films lead to high Faradaic efficiency 86.5% full-cell electricity conversion 36.5% towards C2+ flow cell. By further scaling up electrode into 25 cm2 membrane assembly system, overall current...

The mechanism of how interfacial wettability impacts the CO2 electroreduction pathways to ethylene and ethanol remains unclear. This paper describes design realization controllable equilibrium kinetic-controlled *CO *H via modifying alkanethiols with different alkyl chain lengths reveal its contribution pathways. Characterization simulation that mass transport H2O is related wettability, which may result in variation ratio, affects Through modulating hydrophilic interface superhydrophobic...

Acidic electrochemical CO2 reduction reaction (CO2RR) can minimize carbonate formation and eliminate crossover, thereby improving long-term stability enhancing single-pass carbon efficiency (SPCE). However, the kinetically favored hydrogen evolution (HER) is generally predominant under acidic conditions. This paper describes confinement of a local alkaline environment for efficient CO2RR in strongly electrolyte through manipulation mass transfer processes well-designed hollow-structured Ag@C...

This communication describes collaboration between a grain-boundary-mediated Au catalytic layer and TiO₂-protected a-Si absorber towards adjustable PEC syngas production with low onset potentials.

Carbon dioxide (CO2 ) reduction in aqueous solutions is an attractive strategy for carbon capture and utilization. Cuprous oxide (Cu2 O) a promising catalyst CO2 as it can convert into valuable hydrocarbons suppress the side hydrogen evolution reaction (HER). However, nature of active sites Cu2 O remains under debate because complex surface structure reducing conditions, leading to limited guidance designing improved catalysts. This paper describes functionality surface-bonded hydroxy groups...

Abstract The reduction of carbon dioxide using electrochemical cells is an appealing technology to store renewable electricity in a chemical form. preferential adsorption oxygen over atoms intermediates could improve the methanol selectivity due retention C–O bond. However, adsorbent-surface interaction mainly related d states transition metals catalysts, thus it difficult promote formation oxygen-bound without affecting affinity. This paper describes construction molybdenum-based metal...

The electrochemical CO2 reduction (CO2 ER) to multi-carbon chemical feedstocks over Cu-based catalysts is of considerable attraction but suffers with the ambiguous nature active sites, which hinder rational design and large-scale industrialization. This paper describes a simulation obtain realistic CuZn nanoparticle models atom-level structure sites for C2+ products on in ER, combining neural network based global optimization density functional theory calculations. Upon analyzing 2000...

Photoelectrochemical CO2 reduction reaction flow cells are promising devices to meet the requirements produce solar fuels at industrial scale. Photoelectrodes with wide bandgaps do not allow for efficient high current densities, while integration of opaque photoelectrodes narrow in cell configurations still remains a challenge. This paper describes design and fabrication back-illuminated Si photoanode promoted PEC reaction. The illumination area catalytic sites photoelectrode decoupled,...

In the electrochemical CO

Abstract Photoelectrochemical seawater splitting is a promising route for direct utilization of solar energy and abundant resources H 2 production. However, the complex salinity composition in results intractable challenges photoelectrodes. This paper describes fabrication bilayer stack consisting stainless steel TiO as cocatalyst protective layer Si photoanode. The chromium-incorporated NiFe (oxy)hydroxide converted from film serves efficient oxygen evolution retarding adsorption corrosive...

Abstract It is of great significance to reveal the detailed mechanism neighboring effects between monomers, as they could not only affect intermediate bonding but also change reaction pathway. This paper describes electronic effect Zn/Co monomers effectively promoting CO 2 electroreduction CO. Zn and Co atoms coordinated on N doped carbon (ZnCoNC) show a faradaic efficiency 93.2 % at −0.5 V versus RHE during 30‐hours test. Extended X‐ray absorption fine structure measurements (EXAFS)...

Gas diffusion electrodes (GDEs) mediate the transport of reactants, products and electrons for electrocatalytic CO

Abstract Copper can efficiently electro‐catalyze carbon dioxide reduction to C 2+ products (C 2 H 4 , 5 OH, n‐propanol). However, the correlation between activity and active sites remains ambiguous, impeding further improvements in their performance. The facet effect of copper crystals promote CO adsorption C−C coupling consequently yield a superior selectivity for is described. We achieve high Faradaic efficiency (FE) 87 % large partial current density 217 mA cm −2 toward on Cu(OH) ‐D at...

The grain boundaries (GBs) in copper (Cu) electrocatalysts have been suggested as active sites for CO2 electroreduction to ethanol. Nevertheless, the mechanisms are still elusive. Herein, we describe how GBs tune activity and selectivity ethanol on two representative Cu-GB models, namely Cu∑3/(111) GB Cu∑5/(100) GB, using joint first-principles calculations experiments. unique geometric structures facilitate adsorption of bidentate intermediates, *COOH *CHO, which crucial activation CO...

The electroreduction of CO2 plays an important role in achieving a net-zero carbon economy. Imidazolium cations can be used to enhance the rate reduction reactions, but origin this promotion remains poorly understood. In work, we show that presence 1-ethyl-3-methylimidazolium (EMIM+), on Ag electrodes occurs with apparent activation energy near zero, while applied potential influences through pre-exponential factor. Our findings suggest is controlled by initial state entropy, which depends...

ConspectusAs one of the essential pathways to carbon neutrality or negativity, electrochemical reduction CO2 offers tremendous prospects for platform chemicals and fuel production. Copper (Cu) is currently only metal material that able reduce multicarbon (C2+) products. Despite fact copper-based materials have been investigated decades, we still confront numerous challenges on path fundamental understanding large-scale deployment electrocatalysts reduction. For investigations, it remains a...

Abstract Electroreductive coupling of biomass-derived benzaldehyde offers a sustainable approach to producing value-added hydrobenzoin. The low efficiency the reaction mainly ascribes mismatch initial formation and subsequent dimerization ketyl intermediates (Ph-CH = O → Ph-C·-OH Ph-C(OH)-C(OH)-Ph). This paper describes strategy balance active sites for generation by constructing bimetallic Pd/Cu electrocatalysts with tunable surface coverage Pd. A Faradaic 63.2% hydrobenzoin production rate...

Abstract Photoelectrochemical (PEC) seawater splitting is a promising method for the direct utilization of solar energy and abundant resources hydrogen production. Photoelectrodes are susceptible to various ions in complicated competitive reactions, resulting failure photoelectrodes. This paper proposes design fabrication different sputtered stainless steel (SS) films deposited on silicon photoanodes, completely isolating electrolytes semiconductor substrate. Upon coupling with PEC flow...