Approaching a high-rate and sustainable production of hydrogen peroxide: oxygen reduction on Co–N–C single-atom electrocatalysts in simulated seawater

Energy & Environmental Science, Journal Year: 2021, Volume and Issue: 14(10), P. 5444 - 5456

Published: Jan. 1, 2021

Sustainable production of H 2 O is boosted by oxygen reduction reaction on Co–N 5 sites in a flow cell simulated seawater.

Language: Английский

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Progress of Electrochemical Hydrogen Peroxide Synthesis over Single Atom Catalysts

ACS Materials Letters, Journal Year: 2020, Volume and Issue: 2(8), P. 1008 - 1024

Published: July 9, 2020

The electrochemical oxygen reduction reaction (ORR) via the two-electron pathway provides a promising approach for direct synthesis of hydrogen peroxide (H2O2) and its on-site utilizations. effective electrocatalyst is one key factors determining future applications this technology. In recent years, various catalysts, such as pristine carbon materials, modified materials (oxidized or heteroatom doped nitrogen, fluorine, sulfur doped), gold, mercury alloyed palladium platinum nanoparticles, well transition metal single atom catalysts (SACs) have been reported to effectively catalyze H2O2 production ORR process. Among these candidates, SACs with 100% utilization well-defined active centers attracted extra attention due their high catalytic performance synthesis. review, thermodynamics, molecular activation, theoretical screening prediction are discussed. performance, kinetics mechanism together devices summarized. It hoped that contribution can offer comprehensive reference progress in

Language: Английский

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The effect of coordination environment on the activity and selectivity of single-atom catalysts

Coordination Chemistry Reviews, Journal Year: 2022, Volume and Issue: 461, P. 214493 - 214493

Published: March 10, 2022

Language: Английский

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A Machine Learning Model on Simple Features for CO₂ Reduction Electrocatalysts

The Journal of Physical Chemistry C, Journal Year: 2020, Volume and Issue: 124(41), P. 22471 - 22478

Published: Sept. 16, 2020

Electroreduction of CO2 is one the most potential ways to realize recycle and energy regeneration. The key promoting this technology development high-performance electrocatalysts. Generally, high-throughput computational screening contributes a lot materials innovation, but still consumes much time resource. To achieve efficient exploration electrocatalysts for reduction, we created machine learning model based on an extreme gradient boosting regression (XGBR) algorithm simple features. Our successfully rapidly predicted Gibbs free change CO adsorption (ΔGCO) 1060 atomically dispersed metal–nonmetal codoped graphene systems, greatly reduced research cost. competitive reaction, hydrogen evolution reaction (HER), also discussed with respect such model. This work demonstrates methods provides convenient approach effective theoretical design reduction.

Language: Английский

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Fe₁N₄–O₁ site with axial Fe–O coordination for highly selective CO₂ reduction over a wide potential range

Energy & Environmental Science, Journal Year: 2021, Volume and Issue: 14(6), P. 3430 - 3437

Published: Jan. 1, 2021

The proposed working mechanism of the electrochemical CO₂ reduction reaction on Fe₁N₄, Fe₁N₄–N₁, and Fe₁N₄–O₁ active sites.

Language: Английский

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Facile Top-Down Strategy for Direct Metal Atomization and Coordination Achieving a High Turnover Number in CO₂ Photoreduction

Journal of the American Chemical Society, Journal Year: 2020, Volume and Issue: 142(45), P. 19259 - 19267

Published: Oct. 29, 2020

Developing unique single atoms as active sites is vitally important to boosting the efficiency of photocatalytic CO2 reduction, but directly atomizing metal particles and simultaneously adjusting configuration individual remain challenging. Herein, we demonstrate a facile strategy at relatively low temperature (500 °C) access in situ atomization coordination adjustment via thermo-driven gaseous acid. Using this strategy, pyrolytic acid (HCl) from NH4Cl could downsize large into corresponding ions, which subsequently anchored onto surface defects nitrogen-rich carbon (NC) matrix. Additionally, low-temperature treatment-induced C═O motifs within interlayer NC bond with discrete Fe perpendicular direction finally create stabilized Fe-N4O species high valence status (Fe3+) on shallow It was found that can achieve highly efficient conversion when accepting energetic electrons both homogeneous heterogeneous photocatalysts. The optimized sample achieves maximum turnover number (TON) 1494 1 h CO generation selectivity 86.7% well excellent stability. Experimental theoretical results unravel promote adsorption lower formation barrier key intermediate COOH* compared traditional Fe-N4 moiety chemical valence. Our discovery provides new points view construction more single-atom cocatalysts by considering optimization atomic for high-performance photoreduction.

Language: Английский

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Tuning Two‐Electron Oxygen‐Reduction Pathways for H₂O₂ Electrosynthesis via Engineering Atomically Dispersed Single Metal Site Catalysts

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(23)

Published: Feb. 8, 2022

Abstract The hydrogen peroxide (H 2 O ) generation via the electrochemical oxygen reduction reaction (ORR) under ambient conditions is emerging as an alternative and green strategy to traditional energy‐intensive anthraquinone process unsafe direct synthesis using H . It enables on‐site decentralized production air renewable electricity for various applications. Currently, atomically dispersed single metal site catalysts have emerged most promising platinum group (PGM)‐free electrocatalysts ORR. Further tuning their central sites, coordination environments, local structures can be highly active selective 2e − Herein, recent methodologies achievements on developing are summarized. Combined with theoretical computation advanced characterization, a structure–property correlation guide rational catalyst design favorable ORR aimed provide. Due oxidative nature of derived free radicals, stability effective solutions improve tolerance emphasized. Transferring intrinsic properties electrode performance viable applications always remains grand challenge. key metrics knowledge during electrolyzer development are, therefore, highlighted.

Language: Английский

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Recent Developments of Microenvironment Engineering of Single‐Atom Catalysts for Oxygen Reduction toward Desired Activity and Selectivity

Advanced Functional Materials, Journal Year: 2021, Volume and Issue: 31(45)

Published: Aug. 7, 2021

Abstract Oxygen reduction reaction (ORR) is an essential process for sustainable energy supply and sufficient chemical production in modern society. Single‐atom catalysts (SACs) exhibit great potential on maximum atomic efficiency, high ORR activity, stability, making them attractive candidates pursuing next‐generation catalysts. Despite substantial efforts being made building diversiform single‐atom active sites (SAASs), the performance of obtained still unsatisfactory. Fortunately, microenvironment regulation SACs provides opportunities to improve activity selectivity ORR. In this review, first, mechanism pathways N‐coordinated SAAS, electrochemical evaluation, characterization SAAS are displayed. addition, recent developments tuning systematically summarized, especially, strategies modulation introduced detail boosting intrinsic 4e − /2e selectivity. Theoretical calculations cutting‐edge techniques united discussed fundamental understanding synthesis–construction–performance correlations. Furthermore, their comprehensively overviewed acquire outstanding SACs. Lastly, by proposing perspectives remaining challenges infant engineering, future directions other analogous procedures pointed out.

Language: Английский

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Template-Sacrificing Synthesis of Well-Defined Asymmetrically Coordinated Single-Atom Catalysts for Highly Efficient CO₂ Electrocatalytic Reduction

ACS Nano, Journal Year: 2022, Volume and Issue: 16(2), P. 2110 - 2119

Published: Feb. 11, 2022

Although various single-atom catalysts have been designed, atomically engineering their coordination environment remains a great challenge. Herein, one-pot template-sacrificing pyrolysis approach is developed to synthesize well-defined Ni-N4-O catalytic sites on highly porous graphitic carbon for electrocatalytic CO2 reduction CO with high Faradaic efficiency (maximum of 97.2%) in wide potential window (-0.56 -1.06 V vs RHE) and stability. In-depth experimental theoretical studies reveal that the axial Ni-O introduces asymmetry center, leading lower Gibbs free energy rate-limiting step, strengthened binding *COOH, weaker association *CO. The present results demonstrate successful atomic-level high-surface-area carbon-supported Ni (SACs), demonstrated method can be applied an array SACs (metal-N4-O) catalysis applications.

Language: Английский

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Rational design of heterogenized molecular phthalocyanine hybrid single-atom electrocatalyst towards two-electron oxygen reduction

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: March 14, 2023

Abstract Single-atom catalysts supported on solid substrates have inspired extensive interest, but the rational design of high-efficiency single-atom is still plagued by ambiguous structure determination active sites and its local support effect. Here, we report hybrid an axial coordination linkage molecular cobalt phthalocyanine with carbon nanotubes for selective oxygen reduction reaction screening from a series metal phthalocyanines via preferential density-functional theory calculations. Different conventional heterogeneous catalysts, are proven to facilitate target as well understanding underlying mechanism due well-defined site clear in catalysts. Consequently, optimized Co exhibit improved 2e − performance compared corresponding homogeneous catalyst terms activity selectivity. When prepared air cathode air-breathing flow cell device, enable at 300 mA cm −2 exhibiting stable Faradaic efficiency exceeding 90% 25 h.

Language: Английский

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