Bismuth Iron Oxide Catalysts for Efficient CO Electroreduction to Formate.

Renewable energy-driven electrocatalytic CO reduction reaction (CORR) over bismuth-based catalysts shows great promise for converting CO into formic acid and formate while closing the carbon cycle. Herein, we report a high-performance BiFeO/BiFeO precatalyst, which delivers a formate partial current density of 359.8 mA cm and a formate formation rate of 6.

CO electrolysis to multicarbon products over grain boundary-rich Cu nanoparticles in membrane electrode assembly electrolyzers.

Producing valuable chemicals like ethylene via catalytic carbon monoxide conversion is an important nonpetroleum route. Here we demonstrate an electrochemical route for highly efficient synthesis of multicarbon (C) chemicals from CO. We achieve a C partial current density as high as 4.

Boosting Electrocatalytic Ethylene Epoxidation by Single Atom Modulation.

The electrochemical synthesis of ethylene oxide (EO) using ethylene and water under ambient conditions presents a low-carbon alternative to existing industrial production process. Yet, the electrocatalytic ethylene epoxidation route is currently hindered by largely insufficient activity, EO selectivity, and long-term stability. Here we report a single atom Ru-doped hollandite structure KIrO (KIrRuO) nanowire catalyst for efficient EO production via a chloride-mediated ethylene epoxidation process.

Directing the Selectivity of CO Electrolysis to Acetate by Constructing Metal-Organic Interfaces.

Electrochemically converting CO to valuable chemicals holds great promise for closing the anthropogenic carbon cycle. Owing to complex reaction pathways and shared rate-determining steps, directing the selectivity of CO /CO electrolysis to a specific multicarbon product is very challenging. We report here a strategy for highly selective production of acetate from CO electrolysis by constructing metal-organic interfaces.

Reaction-induced iodine adsorption on Cu surfaces facilitates electrocatalytic CO2 reduction.

The electrolyte effect has been key to the electrochemical CO2 reduction reaction (CO2RR) and has received extensive attention in recent years. Here we combined atomic force microscopy, quasi-in situ X-ray photoelectron spectroscopy, and in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) to study the effect of iodine anions on Cu-catalyzed CO2RR in the absence or presence of KI in the KHCO3 solution. Our results suggested that iodine adsorption caused coarsening of the Cu surface and altered its intrinsic activity for CO2RR.

The Role of Interfacial Water in CO Electrolysis over Ni-N-C Catalyst in a Membrane Electrode Assembly Electrolyzer.

CO electrolysis is a promising route for achieving net-zero emission through decarbonization. To realize CO electrolysis toward practical application, beyond catalyst structures, it is also critical to rationally manipulate catalyst microenvironments such as the water at the electrode/electrolyte interface. Here, the role of interfacial water in CO electrolysis over Ni-N-C catalyst modified with different polymers is investigated.

Coverage-driven selectivity switch from ethylene to acetate in high-rate CO/CO electrolysis.

Tuning catalyst microenvironments by electrolytes and organic modifications is effective in improving CO electrolysis performance. An alternative way is to use mixed CO/CO feeds from incomplete industrial combustion of fossil fuels, but its effect on catalyst microenvironments has been poorly understood. Here we investigate CO/CO co-electrolysis over CuO nanosheets in an alkaline membrane electrode assembly electrolyser.

A Reconstructed Cu P O Catalyst for Selective CO Electroreduction to Multicarbon Products.

The electrochemical CO reduction reaction (CO RR) over Cu-based catalysts shows great potential for converting CO into multicarbon (C ) fuels and chemicals. Herein, we introduce an A M O structure into a Cu-based catalyst through a solid-state reaction synthesis method. The Cu P O catalyst is electrochemically reduced to metallic Cu with a significant structure evolution from grain aggregates to highly porous structure under CO RR conditions.

Asymmetric Oxo-Bridged ZnPb Bimetallic Electrocatalysis Boosting CO -to-HCOOH Reduction.

Electrochemical CO reduction (ECR) is one of the promising CO recycling technologies sustaining the natural carbon cycle and offering more sustainable higher-energy chemicals. Zn- and Pb-based catalysts have improved formate selectivity, but they suffer from relatively low current activities considering the competitive CO selectivity on Zn. Here, lead-doped zinc (Zn(Pb)) electrocatalyst is optimized to efficiently reduce CO to formate, while CO evolution selectivity is largely controlled.

High-Rate CO Electroreduction to C Products over a Copper-Copper Iodide Catalyst.

Electrochemical CO reduction reaction (CO RR) to multicarbon hydrocarbon and oxygenate (C ) products with high energy density and wide availability is of great importance, as it provides a promising way to achieve the renewable energy storage and close the carbon cycle. Herein we design a Cu-CuI composite catalyst with abundant Cu /Cu interfaces by physically mixing Cu nanoparticles and CuI powders. The composite catalyst achieves a remarkable C partial current density of 591 mA cm at -1.

Benzoic Anhydride as a Bifunctional Electrolyte Additive for Hydrogen Fluoride Capture and Robust Film Construction over High-Voltage Li-Ion Batteries.

High-voltage LiNi Co Mn O (NCM811)-based Li-ion batteries (LIBs) with enhanced performance can be achieved by properly tailoring the electrolyte systems. Benzoic anhydride (BA) was proposed here as a promising bifunctional electrolyte additive that can not only construct a robust cathode-electrolyte interface (CEI) film on the electrode surface but also capture HF/H O in the electrolyte effectively. Compared to the cell without the BA additive, the capacity of Li/NCM811 half-cell with 1.

On the Activity/Selectivity and Phase Stability of Thermally Grown Copper Oxides during the Electrocatalytic Reduction of CO.

Revealing the active nature of oxide-derived copper is of key importance to understand its remarkable catalytic performance during the cathodic CO reduction reaction (CORR) to produce valuable hydrocarbons. Using advanced spectroscopy, electron microscopy, and electrochemically active surface area characterization techniques, the electronic structure and the changes in the morphology/roughness of thermally oxidized copper thin films were revealed during CORR. For this purpose, we developed an in situ cell for X-ray spectroscopy that could be operated accurately in the presence of gases or liquids to clarify the role of the initial thermal oxide phase and its active phase during the electrocatalytic reduction of CO.

Enhancing CO Electroreduction to Methane with a Cobalt Phthalocyanine and Zinc-Nitrogen-Carbon Tandem Catalyst.

Developing copper-free catalysts for CO conversion into hydrocarbons and oxygenates is highly desirable for electrochemical CO reduction reaction (CO RR). Herein, we report a cobalt phthalocyanine (CoPc) and zinc-nitrogen-carbon (Zn-N-C) tandem catalyst for CO RR to CH . This tandem catalyst shows a more than 100 times enhancement of the CH /CO production rate ratio compared with CoPc or Zn-N-C alone.

Revealing the Active Phase of Copper during the Electroreduction of CO in Aqueous Electrolyte by Correlating X-ray Spectroscopy and Electron Microscopy.

The variation in the morphology and electronic structure of copper during the electroreduction of CO into valuable hydrocarbons and alcohols was revealed by combining surface- and bulk-sensitive X-ray spectroscopies with electrochemical scanning electron microscopy. These experiments proved that the electrified interface surface and near-surface are dominated by reduced copper. The selectivity to the formation of the key C-C bond is enhanced at higher cathodic potentials as a consequence of increased copper metallicity.

In Situ Reconstruction of a Hierarchical Sn-Cu/SnO Core/Shell Catalyst for High-Performance CO Electroreduction.

The electrochemical CO reduction reaction (CO RR) to give C (formate and CO) products is one of the most techno-economically achievable strategies for alleviating CO emissions. Now, it is demonstrated that the SnO shell in Sn Cu catalyst with a hierarchical Sn-Cu core can be reconstructed in situ under cathodic potentials of CO RR. The resulting Sn Cu catalyst achieves a high current density of 406.

In Situ Investigation of Reversible Exsolution/Dissolution of CoFe Alloy Nanoparticles in a Co-Doped Sr Fe Mo O Cathode for CO Electrolysis.

Reversible exsolution and dissolution of metal nanoparticles in perovskite has been investigated as an efficient strategy to improve CO electrolysis performance. However, fundamental understanding with regard to the reversible exsolution and dissolution of metal nanoparticles in perovskite is still scarce. Herein, in situ exsolution and dissolution of CoFe alloy nanoparticles in Co-doped Sr Fe Mo O (SFMC) revealed by in situ X-ray diffraction, scanning transmission electron microscopy, environmental scanning electron microscopy, and density functional theory calculations are reported.

Structure- and Electrolyte-Sensitivity in CO Electroreduction.

The utilization of fossil fuels (i.e., coal, petroleum, and natural gas) as the main energy source gives rise to serious environmental issues, including global warming caused by the continuously increasing level of atmospheric CO.

Dynamic Changes in the Structure, Chemical State and Catalytic Selectivity of Cu Nanocubes during CO Electroreduction: Size and Support Effects.

In situ and operando spectroscopic and microscopic methods were used to gain insight into the correlation between the structure, chemical state, and reactivity of size- and shape-controlled ligand-free Cu nanocubes during CO electroreduction (CO RR). Dynamic changes in the morphology and composition of Cu cubes supported on carbon were monitored under potential control through electrochemical atomic force microscopy, X-ray absorption fine-structure spectroscopy and X-ray photoelectron spectroscopy. Under reaction conditions, the roughening of the nanocube surface, disappearance of the (100) facets, formation of pores, loss of Cu and reduction of CuO species observed were found to lead to a suppression of the selectivity for multi-carbon products (i.

Electrochemical promotion of catalysis over Pd nanoparticles for CO reduction.

Electrochemical promotion of catalysis (EPOC) has been shown to accelerate the rate of many heterogeneous catalytic reactions; however, it has rarely been reported in low-temperature aqueous electrochemical reactions. Herein, we report a significant EPOC effect for the CO reduction to generate formate over Pd nanoparticles (NPs) in a 1 M KHCO aqueous solution. By applying a negative potential over differently-sized Pd NPs, the rate of formate production is greatly improved as compared to that at an open-circuit voltage, with a rate enhancement ratio ranging from 10 to 143.

Plasma-Activated Copper Nanocube Catalysts for Efficient Carbon Dioxide Electroreduction to Hydrocarbons and Alcohols.

Carbon dioxide electroreduction to chemicals and fuels powered by renewable energy sources is considered a promising path to address climate change and energy storage needs. We have developed highly active and selective copper (Cu) nanocube catalysts with tunable Cu(100) facet and oxygen/chlorine ion content by low-pressure plasma pretreatments. These catalysts display lower overpotentials and higher ethylene, ethanol, and n-propanol selectivity, resulting in a maximum Faradaic efficiency (FE) of ∼73% for C and C products.

Enhancing CO Electroreduction with the Metal-Oxide Interface.

The electrochemical CO reduction reaction (CORR) typically uses transition metals as the catalysts. To improve the efficiency, tremendous efforts have been dedicated to tuning the morphology, size, and structure of metal catalysts and employing electrolytes that enhance the adsorption of CO. We report here a strategy to enhance CORR by constructing the metal-oxide interface.

Correction: Electrochemical promotion of catalysis over Pd nanoparticles for CO reduction.

[This corrects the article DOI: 10.1039/C6SC04966D.].

Size-dependent electrocatalytic reduction of CO2 over Pd nanoparticles.

Size effect has been regularly utilized to tune the catalytic activity and selectivity of metal nanoparticles (NPs). Yet, there is a lack of understanding of the size effect in the electrocatalytic reduction of CO2, an important reaction that couples with intermittent renewable energy storage and carbon cycle utilization. We report here a prominent size-dependent activity/selectivity in the electrocatalytic reduction of CO2 over differently sized Pd NPs, ranging from 2.