Electroreduction of CO into valuable chemicals and fuels is a promising strategy to mitigate energy and environmental problems. However, it usually suffers from unsatisfactory selectivity for a single product and inadequate electrochemical stability. Herein, we report the first work to use cationic Gemini surfactants as modifiers to boost CO electroreduction to formate.
View Article and Find Full Text PDFElectrochemical reduction reaction of carbon monoxide (CORR) offers a promising way to manufacture acetic acid directly from gaseous CO and water at mild condition. Herein, we discovered that the graphitic carbon nitride (g-C N ) supported Cu nanoparticles (Cu-CN) with the appropriate size showed a high acetate faradaic efficiency of 62.8 % with a partial current density of 188 mA cm in CORR.
View Article and Find Full Text PDFAmorphous nano-metal catalysts often exhibit appealing catalytic properties, because the intrinsic linear scaling relationship can be broken. However, accurate control synthesis of amorphous nano-metal catalysts with desired size and morphology is a challenge. In this work, we discover that Cu(0) could be oxidized to amorphous CuO species by supercritical CO.
View Article and Find Full Text PDFCurrent techno-economic evaluation manifests that the electrochemical CO reduction reaction (eCORR) to CO is very promising considering its simple two-electron transfer process, minimum cost of electricity, and low separation cost. Herein, we report a Sn-modification strategy that can tune the local electronic structure of Cu with an appropriate valence. The as-prepared catalysts can alter the broad product distribution of Cu-based eCORR to predominantly generate CO.
View Article and Find Full Text PDFThe electroreduction of CO to CH has attracted extensive attention. However, it is still a challenge to achieve high current density and faradaic efficiency (FE) for producing CH because the reaction involves eight electrons and four protons. In this work, we designed Cu nanoparticles supported on N-doped carbon (Cu-np/NC).
View Article and Find Full Text PDFOxide-derived copper (OD-Cu) has been discovered to be an effective catalyst for the electroreduction of CO to C2+ products. The structure of OD-Cu and its surface species during the reaction process are interesting topics, which have not yet been clearly discussed. Herein, surface-enhanced Raman spectroscopy (SERS), operando X-ray absorption spectroscopy (XAS), and O isotope labeling experiments were employed to investigate the surface species and structures of OD-Cu catalysts during CO electroreduction.
View Article and Find Full Text PDFElectroreduction of CO into valuable fuels and feedstocks offers a promising way for CO utilization. However, the commercialization is limited by the low productivity. Here, we report a strategy to enhance the productivity of CO electroreduction by improving diffusion of CO to the surface of catalysts using porous organic cages (POCs) as an additive.
View Article and Find Full Text PDFIt is very interesting to synthesize high value-added chemicals from CO under mild conditions with low energy consumption. Here, we report that a novel catalyst, Zn(betaine)Br, can efficiently promote the cycloaddition of CO with epoxides to synthesize cyclic carbonates under ambient conditions (30 °C, 1 atm). DFT calculations provide important insights into the mechanism, particularly the unusual synergistic catalytic action of Zn, Br and NR, which is the critical factor for the outstanding performance of Zn(betaine)Br.
View Article and Find Full Text PDFPowered by a renewable electricity source, electrochemical CO reduction reaction is a promising solution to facilitate the carbon balance. However, it is still a challenge to achieve a desired product with commercial current density and high efficiency. Herein we designed quasi-square-shaped cadmium hydroxide nanocatalysts for CO electroreduction to CO.
View Article and Find Full Text PDFUsing renewable electricity to drive CO electroreduction is an attractive way to achieve carbon-neutral energy cycle and produce value-added chemicals and fuels. As an important platform molecule and clean fuel, methanol requires 6-electron transfer in the process of CO reduction. Currently, CO electroreduction to methanol suffers from poor efficiency and low selectivity.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2021
Guided by first-principles calculations, it was found that Cd single-atom catalysts (SACs) have excellent performance in activating CO , and the introduction of axial coordination structure to Cd SACs cannot only further decrease the free energy barrier of CO reduction, but also suppress the hydrogen evolution reaction (HER). Based on the above discovery, we designed and synthesized a novel Cd SAC that comprises an optimized CdN S moiety incorporated in a carbon matrix. It was shown that the catalyst exhibited outstanding performance in CO electroreduction to CO.
View Article and Find Full Text PDFElectrocatalytic reduction of CO into multicarbon (C) products powered by renewable electricity offers one promising method for CO utilization and promotes the storage of renewable energy under an ambient environment. However, there is still a dilemma in the manufacture of valuable C products between balancing selectivity and activity. In this work, cerium oxides were combined with CuO (CeO/CuO) and showed an outstanding catalytic performance for C products.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2020
Electroreduction of CO to liquid fuels such as ethanol and n-propanol, powered by renewable electricity, offers a promising strategy for controlling the global carbon balance and addressing the need for the storage of intermittent renewable energy. In this work, we discovered that the composite composed of nitrogen-doped graphene quantum dots (NGQ) on CuO-derived Cu nanorods (NGQ/Cu-nr) was an outstanding electrocatalyst for the reduction of CO to ethanol and n-propanol. The Faradaic efficiency (FE) of C2+ alcohols could reach 52.
View Article and Find Full Text PDFElectroreduction of CO to CO powered by renewable electricity is a possible alternative to synthesizing CO from fossil fuel. However, it is very hard to achieve high current density at high faradaic efficiency (FE). Here, the first use of N,P-co-doped carbon aerogels (NPCA) to boost CO reduction to CO is presented.
View Article and Find Full Text PDFSingle-atom catalysts (SACs) exhibit intriguing catalytic performance owing to their maximized atom utilizations and unique electronic structures. However, the reported strategies for synthesizing SACs generally have special requirements for either the anchored metals or the supports. Herein, we report a universal approach of electrochemical deposition that is applicable to a wide range of metals and supports for the fabrication of SACs.
View Article and Find Full Text PDFThe development of highly efficient oxygen-evolving catalysts compatible with powerful proton-exchange-membrane-based electrolyzers in acid environments is of prime importance for sustainable hydrogen production. In this field, understanding the role of electronic structure of catalysts on catalytic activity is essential but still lacking. Herein, a family of pyrochlore oxides R Ir O (R = rare earth ions) is reported as acidic oxygen-evolving catalysts with superior-specific activities.
View Article and Find Full Text PDFFinding an active and durable catalyst for the acidic oxygen reduction reaction (ORR), a key process for fuel cells, remains an open challenge due to the thermodynamically contradictory requirements for activity and durability. Here, we report that an active and durable ORR catalyst can be achieved by integrating multiple structural and compositional advantages into one catalyst. The mass activity and specific activity of as-obtained 1-nm-thick PtNiRh trimetallic nanowires/C catalyst were 15.
View Article and Find Full Text PDFExploring efficient and economical electrocatalysts for hydrogen evolution reaction is of great significance for water splitting on an industrial scale. Tungsten oxide, WO, has been long expected to be a promising non-precious-metal electrocatalyst for hydrogen production. However, the poor intrinsic activity of this material hampers its development.
View Article and Find Full Text PDFIn the present work, a highly sensitive and selective biosensor based on aptamer-functionalized nanoporous gold film (NPGF) was successfully developed for direct electrochemical detection of bisphenol A (BPA). NPGF was prepared by dealloying Ag from Au/Ag alloy leaf in concentrated nitric acid. The obtained NPGF was attached onto glassy carbon electrode and then was functionalized with BPA-specific aptamer via the formation of Au-S bond.
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