pH‐Universal Electrocatalytic CO₂ Reduction with Ampere‐Level Current Density on Doping‐Engineered Bismuth Sulfide

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(32)

Published: May 27, 2024

Abstract The practical application of the electrocatalytic CO 2 reduction reaction (CO RR) to form formic acid fuel is hindered by limited activation molecules and lack universal feasibility across different pH levels. Herein, we report a doping‐engineered bismuth sulfide pre‐catalyst (BiS‐1) that S partially retained after electrochemical reconstruction into metallic Bi for RR formate/formic with ultrahigh performance wide range. best BiS‐1 maintains Faraday efficiency (FE) ~95 % at 2000 mA cm −2 in flow cell under neutral alkaline solutions. Furthermore, catalyst shows unprecedentedly high FE (~95 %) current densities from 100 1300 acidic Notably, density can reach 700 while maintaining above 90 membrane electrode assembly electrolyzer operate stably 150 h 200 . In situ spectra functional theory calculations reveals doping modulates electronic structure effectively promotes formation HCOO* intermediate generation. This work develops efficient stable electrocatalysts sustainable production.

Language: Английский

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Cobalt‐Doped Bismuth Nanosheet Catalyst for Enhanced Electrochemical CO₂ Reduction to Electrolyte‐Free Formic Acid

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(36)

Published: June 18, 2024

Electrochemical carbon dioxide (CO

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Oxygen‐Pinned Ag₁In Single‐Atom Alloy for Efficient Electroreduction CO₂ to Formate

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(27)

Published: May 2, 2024

Abstract Catalytic conversion of CO 2 to valuable formate provides a pathway carbon neutrality. Indium (In), as promising catalyst, exhibits high selectivity toward due its suitable bonding ability *OCHO intermediates. However, it still suffers from the activation and protonation steps, leading low activity productivity. Here, an oxygen‐pinned stabilization AgIn single‐atom alloy (O p ‐Ag 1 In) is presented for efficiently converting into (≈92.03% Faradaic efficiency) with partial current density 13 mA cm −2 at −0.95 V vs RHE by using standard H‐type reactor. The O In electrocatalyst more effective in because activated sites catalyst regulate step RR formation sufficient amounts *OCHO, which are confirmed situ spectroscopic theoretical calculations. continuous production showcased 70 –2 24 h utilizing flow cell In.

Language: Английский

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Construction of Low‐Coordination Cu−C₂ Single‐Atoms Electrocatalyst Facilitating the Efficient Electrochemical CO₂ Reduction to Methane

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(49)

Published: Oct. 25, 2023

Constructing Cu single-atoms (SAs) catalysts is considered as one of the most effective strategies to enhance performance electrochemical reduction CO2 (e-CO2 RR) towards CH4 , however there are challenges with activity, selectivity, and a cumbersome fabrication process. Herein, by virtue meta-position structure alkynyl in 1,3,5-triethynylbenzene interaction between -C≡C-, SAs electrocatalyst (Cu-SAs/HGDY), containing low-coordination Cu-C2 active sites, was synthesized through simple efficient one-step method. Notably, this represents first achievement preparing coordination structure, which exhibited high -to-CH4 selectivity (72.1 %) partial current density 230.7 mA cm-2 turnover frequency 2756 h-1 dramatically outperforming currently reported catalysts. Comprehensive experiments calculations verified not only endowed center more positive electricity but also promoted formation H•, contributed outstanding e-CO2 RR electrocatalytic Cu-SAs/HGDY. Our work provides novel H⋅-transferring mechanism for offers protocol preparation two-coordinated

Language: Английский

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InBi Bimetallic Sites for Efficient Electrochemical Reduction of CO₂ to HCOOH

Small, Journal Year: 2023, Volume and Issue: 19(41)

Published: June 13, 2023

Formic acid is receiving intensive attention as being one of the most progressive chemical fuels for electrochemical reduction carbon dioxide. However, majority catalysts suffer from low current density and Faraday efficiency. To this end, an efficient catalyst In/Bi-750 with InOx nanodots load prepared on a two-dimensional nanoflake Bi2 O2 CO3 substrate, which increases adsorption * CO2 due to synergistic interaction between bimetals exposure sufficient active sites. In H-type electrolytic cell, formate efficiency (FE) reaches 97.17% at -1.0 V (vs reversible hydrogen electrode (RHE)) no significant decay over 48 h. A 90.83% also obtained in flow cell higher 200 mA cm-2 . Both in-situ Fourier transform infrared spectroscopy (FT-IR) theoretical calculations show that BiIn bimetallic site can deliver superior binding energy OCHO intermediate, thereby fundamentally accelerating conversion HCOOH. Furthermore, assembled Zn-CO2 exhibits maximum power 6.97 mW cm-1 stability 60

Language: Английский

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Reconstructed Bismuth Oxide through in situ Carbonation by Carbonate‐containing Electrolyte for Highly Active Electrocatalytic CO₂ Reduction to Formate

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(9)

Published: Dec. 26, 2023

The catalyst-reconstruction makes it challenging to clarify the practical active sites and unveil actual reaction mechanism during CO

Language: Английский

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Electrochemistry Enabled Heterostructure with High Tap Density for Ultrahigh Power Na‐Ion Capacitors

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(44)

Published: Oct. 3, 2023

Abstract Developing electrode materials with high tap density, low cost, and superior performance poses a formidable challenge in electrochemistry. The impressive exhibited by most electrodes comes at the expense of density severely limiting their practical applications. Here, combining computational experimental results, an approach for rich heterostructure (Cu 2 S/Na S n ) from cheap copper smelting slag enabled electrochemical process is proposed, reducing diffusion energy barrier 0.82 to 0.28 eV Na + , as well delivering impressively 3.32 g cm −3 . Furthermore, activation that irreversibly generates more stable Cu after first charge progress parent also revealed in/ex situ analytical techniques. As expected, assembled sodium ion capacitors (SICs) achieve (74.4 Wh kg −1 power (20 000 W outstanding capacity retention 81.5% 10 cycles, over 76% its 13.4 s, which surpasses achieved state‐of‐the‐art SICs. This work not only provides novel insights into conversion‐type anodes but introduces method efficient value‐added utilization slag.

Language: Английский

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Electronic structural engineering of bimetallic Bi-Cu alloying nanosheet for highly-efficient CO2 electroreduction and Zn-CO2 batteries

Nano Research, Journal Year: 2023, Volume and Issue: unknown

Published: Nov. 24, 2023

Language: Английский

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Thermal‐Driven Dispersion of Bismuth Nanoparticles among Carbon Matrix for Efficient Carbon Dioxide Reduction

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(28)

Published: April 27, 2024

Abstract The poor electrocatalytic stability and rapid deactivation of metal electrocatalysts are always present in the conversion carbon dioxide (CO 2 ) due to harsh reduction condition. Herein, we demonstrate controllable dispersion ultrafine bismuth nanoparticles among hollow shell (Bi@C‐700‐4) simply by a thermal‐driven diffusion process. confinement effect nitrogen‐doped matrix is able low surface energy against easy aggregation commonly observed for thermal treatment. On basis synergistic between matrix, highly dispersed active sites render obviously improved activity CO into formate. situ experimental observations on process theoretical calculations reveal that incorporation with would promote activation formation key intermediate (*OCHO), thus leading enhanced activity, Faradaic Efficiency (FE) formate about 94.8 % long‐time stability. Furthermore, coupling an anode 5‐hydroxymethylfurfural oxidation reaction (HMFOR) solar‐driven system renders high 2,5‐furandicarboxylic acid (FDCA) yield 81.2 %, presenting impressive solar‐to‐fuel conversion.

Language: Английский

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Deciphering in-situ surface reconstruction in two-dimensional CdPS3 nanosheets for efficient biomass hydrogenation

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: June 18, 2024

Abstract Steering on the intrinsic active site of an electrode material is essential for efficient electrochemical biomass upgrading to valuable chemicals with high selectivity. Herein, we show that in-situ surface reconstruction a two-dimensional layered CdPS 3 nanosheet electrocatalyst, triggered by electrolyte, facilitates 5-hydroxymethylfurfural (HMF) hydrogenation 2,5-bis(hydroxymethyl)furan (BHMF) under ambient condition. The Raman spectroscopy and comprehensive post-mortem catalyst characterizations evidence construction surface-bounded CdS layer form /CdS heterostructure. This electrocatalyst demonstrates promising catalytic activity, achieving Faradaic efficiency BHMF reaching 91.3 ± 2.3 % yield 4.96 0.16 mg/h at − 0.7 V versus reversible hydrogen electrode. Density functional theory calculations reveal generated interface plays pivotal role in optimizing adsorption HMF* H* intermediate, thus facilitating HMF process. Furthermore, reconstructed heterostructure cathode, when coupled MnCo 2 O 4.5 anode, enables simultaneous formate synthesis from glycerol substrates efficiency.

Language: Английский

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