Gas diffusion electrodes (GDEs) for electrochemical reduction of carbon dioxide, carbon monoxide, and dinitrogen to value-added products: a review

Energy & Environmental Science, Journal Year: 2021, Volume and Issue: 14(4), P. 1959 - 2008

Published: Jan. 1, 2021

Opportunities, challenges and design criteria associated with Gas diffusion electrodes (GDEs) for various electrochemical applications.

Language: Английский

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Electrocatalytic CO₂-to-C₂₊ with Ampere-Level Current on Heteroatom-Engineered Copper via Tuning *CO Intermediate Coverage

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(32), P. 14936 - 14944

Published: Aug. 4, 2022

An ampere-level current density of CO2 electrolysis is critical to realize the industrial production multicarbon (C2+) fuels. However, under such a large density, poor CO intermediate (*CO) coverage on catalyst surface induces competitive hydrogen evolution reaction, which hinders reduction reaction (CO2RR). Herein, we report reliable CO2-to-C2+ by heteroatom engineering Cu catalysts. The Cu-based compounds with (N, P, S, O) are electrochemically reduced heteroatom-derived significant structural reconstruction CO2RR conditions. It found that N-engineered (N-Cu) exhibits best productivity remarkable Faradaic efficiency 73.7% -1100 mA cm-2 and an energy 37.2% -900 cm-2. Particularly, it achieves C2+ partial -909 at -1.15 V versus reversible electrode, outperforms most reported In situ spectroscopy indicates adjusts *CO adsorption alters local H proton consumption in solution. Density functional theory studies confirm high strength N-Cu results from depressed HER promoted both bridge atop sites Cu, greatly reduces barrier for C-C coupling.

Language: Английский

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The Critical Impacts of Ligands on Heterogeneous Nanocatalysis: A Review

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(10), P. 6020 - 6058

Published: May 4, 2021

Ligand utilization is a necessary and powerful technique for the colloidal synthesis of nanoparticles (NPs) with controllable sizes regulated morphologies. For catalysis applications, it commonly believed that surface ligands on metal NPs block active catalytic sites reduce activity. Nevertheless, since 2010, an increasing number research groups have demonstrated unexpected benefits improve activity and/or selectivity. These can be ascribed to construction inorganic–organic interface, through which series factors, such as steric, electronic, solubility effects, utilized produce favorable changes interfacial environment. Considering tremendous developments in this emerging field, compile comprehensive systematic overview recent advances. In Review, we summarize critical impacts heterogeneous nanocatalysis. First, introduce vital roles colloid syntheses shapes. Second, detrimental effects nanocatalysis are described basis traditional views. Third, strategies ligand removal reviewed compared. Fourth, has been conducted past decade, three main beneficial (steric, solubility) classified discussed. each effect, possible corresponding mechanism presented, typical examples provided. Recent advances regarding density functional theory (DFT) calculations regulation coverage dedicated explaining ligand-promotion searching optimal nanocatalysts. Fifth, stabilities cutting-edge ligand-capped nanocatalysts before after reactions Finally, highlight remaining challenges propose future perspectives. Although much progress achieved, activities multifaceted still debatable. We hope Review will deepen readers' understanding actual catalysis.

Language: Английский

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High-purity and high-concentration liquid fuels through CO2 electroreduction

Nature Catalysis, Journal Year: 2021, Volume and Issue: 4(11), P. 943 - 951

Published: Nov. 18, 2021

Language: Английский

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Dynamically Formed Surfactant Assembly at the Electrified Electrode–Electrolyte Interface Boosting CO₂ Electroreduction

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(14), P. 6613 - 6622

Published: April 5, 2022

Electrocatalytic reactions occur in the nanoscale space at electrified electrode-electrolyte interface. It is well known that interface, also called as interfacial microenvironment, difficult to investigate due interference of bulk electrolytes and its dynamic evolution response applied bias potential. Here, we employ electrochemical co-reduction CO2 H2O on commercial Ag electrodes a model system, conjunction with quaternary ammonium cationic surfactants electrolyte additives. We probe bias-potential-driven microenvironment mechanistic origin catalytic selectivity. By virtue comprehensive situ vibrational spectroscopy, impedance molecular dynamics simulations, it revealed structure dynamically changed from random distribution nearly ordered assembly increasing The surfactant regulates water environment by repelling isolated suppressing orientation into an promotes enrichment Eventually, formed hydrophobic-aerophilic interface reduces activity dissociation increases selectivity electroreduction CO. These results highlight importance regulating organic additives means boosting performance electrosynthesis beyond.

Language: Английский

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Electrochemical Approaches for CO₂ Conversion to Chemicals: A Journey toward Practical Applications

Accounts of Chemical Research, Journal Year: 2022, Volume and Issue: 55(5), P. 638 - 648

Published: Jan. 18, 2022

ConspectusCarbon capture, utilization, and sequestration play an essential role to address CO2 emissions. Among all carbon utilization technologies, electroreduction has gained immense interest due its potential for directly converting a variety of valuable commodity chemicals using clean, renewable electricity as the sole energy source. The research community witnessed rapid advances in electrolysis technology recent years, including highly selective catalysts, larger-scale reactors, specific process modeling, well mechanistic understanding reduction reaction. field brings promise commercial application rollout chemical manufacturing.This Account focuses on our contributions both fundamental applied electrocatalytic CO reactions. We first discuss (1) development novel electrocatalysts CO2/CO enhance product selectivity lower consumption. Specifically, we synthesized nanoporous Ag homogeneously mixed Cu-based bimetallic catalysts enhanced production from multicarbon products CO, respectively. Then, review efforts (2) reactor engineering, dissolved H-type cell, vapor-fed three-compartment flow membrane electrode assembly, enhancing reaction rates scalability. Next, describe (3) investigation mechanisms situ operando techniques, such surface-enhanced vibrational spectroscopies electrochemical mass spectroscopy. revealed participation bicarbonate Au attenuated total-reflectance infrared absorption spectroscopy, presence "oxygenated" surface Cu under conditions Raman origin oxygen acetaldehyde other electrolyzer spectrometry. Lastly, examine (4) technology, pollutant effects developing techno-economic analysis. SO2 NOx Cu, Ag, Sn catalysts. also identify technical barriers that need be overcome offer perspective accelerating deployment technology.

Language: Английский

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Recent Progresses in Electrochemical Carbon Dioxide Reduction on Copper‐Based Catalysts toward Multicarbon Products

Advanced Functional Materials, Journal Year: 2021, Volume and Issue: 31(37)

Published: June 26, 2021

Abstract Electrochemical carbon dioxide reduction reaction (CO 2 RR) offers a promising way of effectively converting CO to value‐added chemicals and fuels by utilizing renewable electricity. To date, the electrochemical single‐carbon products, especially monoxide formate, has been well achieved. However, efficient conversion more valuable multicarbon products (e.g., ethylene, ethanol, n ‐propanol, ‐butanol) is difficult still under intense investigation. Here, recent progresses in using copper‐based catalysts are reviewed. First, mechanism RR briefly described. Then, representative approaches catalyst engineering introduced toward formation RR, such as composition, morphology, crystal phase, facet, defect, strain, surface interface. Subsequently, key aspects cell for including electrode, electrolyte, design, also discussed. Finally, advances summarized some personal perspectives this research direction provided.

Language: Английский

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Nano-crumples induced Sn-Bi bimetallic interface pattern with moderate electron bank for highly efficient CO2 electroreduction

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: May 5, 2022

CO2 electroreduction reaction offers an attractive approach to global carbon neutrality. Industrial electrolysis towards formate requires stepped-up current densities, which is limited by the difficulty of precisely reconciling competing intermediates (COOH* and HCOO*). Herein, nano-crumples induced Sn-Bi bimetallic interface-rich materials are in situ designed tailored electrodeposition under conditions, significantly expediting production. Compared with bulk alloy pure Sn, this interface pattern delivers optimum upshift Sn p-band center, accordingly moderate valence electron depletion, leads weakened Sn-C hybridization COOH* suitable Sn-O HCOO*. Superior partial density up 140 mA/cm2 for achieved. High Faradaic efficiency (>90%) maintained at a wide potential window durability 160 h. In work, we elevate design highly active stable efficient electroreduction.

Language: Английский

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Durable CO2 conversion in the proton-exchange membrane system

Nature, Journal Year: 2024, Volume and Issue: 626(7997), P. 86 - 91

Published: Jan. 31, 2024

Language: Английский

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Confined Growth of Silver–Copper Janus Nanostructures with {100} Facets for Highly Selective Tandem Electrocatalytic Carbon Dioxide Reduction

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(19)

Published: March 11, 2022

Electrocatalytic carbon dioxide reduction reaction (CO2 RR) holds significant potential to promote neutrality. However, the selectivity toward multicarbon products in CO2 RR is still too low meet practical applications. Here authors report delicate synthesis of three kinds Ag-Cu Janus nanostructures with {100} facets (JNS-100) for highly selective tandem electrocatalytic products. By controlling surfactant and kinetics Cu precursor, confined growth on one six equal faces Ag nanocubes realized. Compared nanocubes, Ag65 -Cu35 JNS-100 demonstrates much superior both ethylene at less negative potentials. Density functional theory calculations reveal that compensating electronic structure monoxide spillover contribute enhanced performance. This study provides an effective strategy design advanced catalysts extensive application RR.

Language: Английский

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