Interfacial assembly of binary atomic metal-Nx sites for high-performance energy devices

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

Published: April 1, 2023

Abstract Anion-exchange membrane fuel cells and Zn–air batteries based on non-Pt group metal catalysts typically suffer from sluggish cathodic oxygen reduction. Designing advanced catalyst architectures to improve the catalyst’s reduction activity boosting accessible site density by increasing loading utilization are potential ways achieve high device performances. Herein, we report an interfacial assembly strategy binary single-atomic Fe/Co-N x with mass loadings through constructing a nanocage structure concentrating high-density Fe/Co–N sites in porous shell. The prepared FeCo-NCH features distribution as 7.9 wt% of around 7.6 × 10 19 g −1 , surpassing most reported M–N catalysts. In anion exchange zinc–air batteries, material delivers peak power densities 569.0 or 414.5 mW cm −2 3.4 2.8 times higher than control devices assembled FeCo-NC. These results suggest that present for promoting catalytic offers new possibilities exploring efficient low-cost electrocatalysts boost performance various energy devices.

Language: Английский

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Atomically Dispersed Ni–Cu Catalysts for pH‐Universal CO₂ Electroreduction

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(13)

Published: Jan. 10, 2023

CO2 electroreduction is of great significance to reduce emissions and complete the carbon cycle. However, unavoidable carbonate formation low utilization efficiency in neutral or alkaline electrolytes hinder its application at commercial scale. The development reduction under acidic conditions provides a promising strategy, but inhibition hydrogen evolution reaction difficult. Herein, first work design Ni-Cu dual atom catalyst supported on hollow nitrogen-doped reported for pH-universal CO. shows high CO Faradaic ≈99% acidic, neutral, electrolytes, partial current densities reach 190 ± 11, 225 10, 489 14 mA cm-2 , respectively. In particular, reaches 64.3%, which twice as that conditions. Detailed study indicates existence electronic interaction between Ni Cu atoms. atoms push d-band center further toward Fermi level, thereby accelerating *COOH. addition, operando characterizations density functional theory calculation are used elucidate possible mechanism electrolytes.

Language: Английский

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Multi-atom cluster catalysts for efficient electrocatalysis

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(21), P. 8923 - 8956

Published: Jan. 1, 2022

This review presents recent developments in the synthesis, modulation and characterization of multi-atom cluster catalysts for electrochemical energy applications.

Language: Английский

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Almost 100 % electron transfer regime over Fe−Co dual-atom catalyst toward pollutants removal: Regulation of peroxymonosulfate adsorption mode

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 339, P. 123178 - 123178

Published: Aug. 15, 2023

Language: Английский

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Inter‐Metal Interaction with a Threshold Effect in NiCu Dual‐Atom Catalysts for CO₂ Electroreduction

Advanced Materials, Journal Year: 2022, Volume and Issue: 35(11)

Published: Nov. 26, 2022

Dual-atom catalysts (DACs) have become an emerging platform to provide more flexible active sites for electrocatalytic reactions with multi-electron/proton transfer, such as the CO2 reduction reaction (CRR). However, introduction of asymmetric dual-atom causes complexity in structure, leaving incomprehensive understanding inter-metal interaction and catalytic mechanism. Taking NiCu DACs example, herein, a rational structural model is proposed, distance-dependent investigated by combining theoretical simulations experiments, including density functional theory computation, aberration-corrected transmission electron microscopy, synchrotron-based X-ray absorption fine Monte Carlo experiments. A distance threshold around 5.3 Å between adjacent NiN4 CuN4 moieties revealed trigger effective electronic regulation boost CRR performance on both selectivity activity. universal macro-descriptor rigorously correlating intrinsic material features (e.g., metal loading thickness) established guide design synthesis advanced DACs. This study highlights significance identifying DACs, helps bridge gap experimental atomically dispersed highly correlated sites.

Language: Английский

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Carbon Nanocage with Maximum Utilization of Atomically Dispersed Iron as Efficient Oxygen Electroreduction Nanoreactor

Advanced Materials, Journal Year: 2022, Volume and Issue: 35(5)

Published: Nov. 9, 2022

As key parameters of electrocatalysts, the density and utilization active sites determine electrocatalytic performance toward oxygen reduction reaction. Unfortunately, prevalent electrocatalysts fail to maximize due inappropriate nanostructural design. Herein, a nano-emulsion induced polymerization self-assembly strategy is employed prepare hierarchical meso-/microporous N/S co-doped carbon nanocage with atomically dispersed FeN4 (denoted as Meso/Micro-FeNSC). In situ scanning electrochemical microscopy technology reveals available for Meso/Micro-FeNSC reach 3.57 × 1014 cm-2 , representing more than threefold improvement compared micropore-dominant Micro-FeNSC counterpart (1.07 ). Additionally, turnover frequency also improved 0.69 from 0.50 e- site-1 s-1 Micro-FeNSC. These properties motivate efficient electroreduction electrocatalyst, in terms outstanding half-wave potential (0.91 V), remarkable kinetic mass specific activity (68.65 A g-1 ), excellent robustness. The assembled Zn-air batteries deliver high peak power (264.34 mW large capacity (814.09 mA h long cycle life (>200 h). This work sheds lights on quantifying site significance maximum rational design advanced catalysts.

Language: Английский

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Improved Electronic Structure from Spin-State Reconstruction of a Heteronuclear Fe–Co Diatomic Pair to Boost the Fenton-like Reaction

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(11), P. 4556 - 4567

Published: March 9, 2023

Dual-atom catalysts (DACs) are promising candidates for various catalytic reactions, including electrocatalysis, chemical synthesis, and environmental remediation. However, the high-activity origin mechanism underlying intrinsic activity enhancement remain elusive, especially Fenton-like reaction. Herein, we systematically compared performance of dual-atom FeCo–N/C with its single-atom counterparts by activating peroxymonosulfate (PMS) pollutant abatement. The unusual spin-state reconstruction on is demonstrated to effectively improve electronic structure Fe Co in d orbital enhance PMS activation efficiency. Accordingly, an intermediate-spin state remarkably boosts reaction almost 1 order magnitude low-spin Co–N/C high-spin Fe–N/C. Moreover, established dual-atom-activated system also exhibits excellent stability robust resistance against harsh conditions. Combined theoretical calculations reveal that unlike unitary atom or transferring electrons molecule, provides extra neighboring positively shifts band center, thereby optimizing adsorption decomposition into a unique high-valent FeIV–O–CoIV species via low-energy barrier pathway. This work advances conceptually novel mechanistic understanding enhanced DACs reactions helps expand application reactions.

Language: Английский

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Recent Progress of Diatomic Catalysts: General Design Fundamentals and Diversified Catalytic Applications

Small, Journal Year: 2022, Volume and Issue: 18(46)

Published: Sept. 23, 2022

Abstract In recent years, some experiments and theoretical work have pointed out that diatomic catalysts not only retain the advantages of monoatomic catalysts, but also introduce a variety interactions, which exceed limit catalytic performance can be applied to many fields. Here, interaction between adjacent metal atoms in is elaborated: synergistic effect, spacing enhancement effect (geometric effect), electronic effect. With regard classification characterization various new are classified into four categories: heteronuclear/homonuclear, with/without carbon carriers, their measures introduced explained detail. aspect preparation widely used atomic layer deposition method, metal–organic framework derivative simple ball milling method introduced, with emphasis on formation mechanism catalysts. Finally, effective control strategies key applications electrocatalysis, photocatalysis, thermal catalysis, other fields given.

Language: Английский

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Promoting Oxygen Reduction Reaction on Atomically Dispersed Fe Sites via Establishing Hydrogen Bonding with the Neighboring P Atoms

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 13(5)

Published: Dec. 16, 2022

Abstract Single atom catalysts (SACs) comprised of nitrogen‐coordinated transition metal (TM–N–C) moieties show encouraging performance towards the oxygen reduction reaction (ORR). Nevertheless, for reactions involving multiple intermediates, single‐atom sites fail to satisfactorily optimize adsorption all intermediates. Here, a facile strategy is reported construct Fe, P dual‐atom in multimodal porous carbon (Fe,P‐DAS@MPC), and its superiority synergistically boosting ORR demonstrated. Fe,P‐DAS@MPC exhibits excellent with substantially positive onset potential ( E = 1.02 V) half‐wave 1/2 0.92 V). Theoretical analysis unveils cooperative effect composed adjacent Fe atoms, aiding hydrogen bonding interaction can promote adsorption/desorption Additionally, Zn–air battery based on shows high peak power density exceptional cycling stability. These findings provide novel avenue design electrocatalysts practical energy conversion applications.

Language: Английский

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Dual Atom Catalysts for Energy and Environmental Applications

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(40)

Published: June 7, 2023

The pursuit of high metal utilization in heterogeneous catalysis has triggered the burgeoning interest various atomically dispersed catalysts. Our aim this review is to assess key recent findings synthesis, characterization, structure-property relationship and computational studies dual-atom catalysts (DACs), which cover full spectrum applications thermocatalysis, electrocatalysis photocatalysis. In particular, combination qualitative quantitative characterization with cooperation DFT insights, synergies superiorities DACs compare counterparts, high-throughput catalyst exploration screening machine-learning algorithms are highlighted. Undoubtably, it would be wise expect more fascinating developments field as tunable

Language: Английский

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