Sustainable zinc–air battery chemistry: advances, challenges and prospects

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(17), P. 6139 - 6190

Published: Jan. 1, 2023

Sustainable zinc-air batteries (ZABs) are considered promising energy storage devices owing to their inherent safety, high density, wide operating temperature window, environmental friendliness, etc., showing great prospect for future large-scale applications. Thus, tremendous efforts have been devoted addressing the critical challenges associated with sustainable ZABs, aiming significantly improve efficiency and prolong operation lifespan. The growing interest in ZABs requires in-depth research on oxygen electrocatalysts, electrolytes, Zn anodes, which not systematically reviewed date. In this review, fundamentals of electrocatalysts air cathodes, physicochemical properties ZAB issues strategies stabilization anodes summarized from perspective fundamental characteristics design principles. Meanwhile, significant advances situ/operando characterization highlighted provide insights into reaction mechanism dynamic evolution electrolyte|electrode interface. Finally, several thoughts perspectives provided regarding opportunities ZABs. Therefore, review provides a thorough understanding advanced chemistry, hoping that timely comprehensive can shed light upcoming horizons prosperous area.

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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Construction of Co₄ Atomic Clusters to Enable Fe−N₄ Motifs with Highly Active and Durable Oxygen Reduction Performance

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(30)

Published: May 24, 2023

Abstract Fe−N−C catalysts with single‐atom Fe−N 4 configurations are highly needed owing to the high activity for oxygen reduction reaction (ORR). However, limited intrinsic and dissatisfactory durability have significantly restrained practical application of proton‐exchange membrane fuel cells (PEMFCs). Here, we demonstrate that constructing adjacent metal atomic clusters (ACs) is effective in boosting ORR performance stability catalysts. The integration uniform Co ACs on N‐doped carbon substrate (Co @/Fe 1 @NC) realized through a “pre‐constrained” strategy using molecular Fe(acac) 3 implanted precursors. as‐developed @NC catalyst exhibits excellent half‐wave potential ( E 1/2 ) 0.835 V vs. RHE acidic media peak power density 840 mW cm −2 H 2 −O cell test. First‐principles calculations further clarify catalytic mechanism identified modified ACs. This work provides viable precisely establishing atomically dispersed polymetallic centers efficient energy‐related catalysis.

Language: Английский

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Regulating the scaling relationship for high catalytic kinetics and selectivity of the oxygen reduction reaction

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

Published: Oct. 27, 2022

The electrochemical oxygen reduction reaction (ORR) is at the heart of modern sustainable energy technologies. However, linear scaling relationship this multistep now becomes bottleneck for accelerating kinetics. Herein, we propose a strategy using intermetallic-distance-regulated atomic-scale bimetal assembly (ABA) that can catalyse direct O‒O radical breakage without formation redundant *OOH intermediates, which could regulate inherent and cause ORR on ABA to follow fast-kinetic dual-sites mechanism. Using in situ synchrotron spectroscopy, directly observe self-adjustable N-bridged Pt = N2 Fe promotes generation key intermediate state (Pt‒O‒O‒Fe) during process, resulting high kinetics selectivity. well-designed catalyst achieves nearly two orders magnitude enhanced kinetic current density half-wave potential 0.95 V relative commercial Pt/C an almost 99% efficiency 4-electron pathway selectivity, making it one catalysts application device zinc‒air cells. This study provides helpful design principle developing optimizing other efficient electrocatalysts.

Language: Английский

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Integration of Alloy Segregation and Surface CoO Hybridization in Carbon‐Encapsulated CoNiPt Alloy Catalyst for Superior Alkaline Hydrogen Evolution

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(41)

Published: July 28, 2023

Abstract Constructing an efficient alkaline hydrogen evolution reaction (HER) catalyst with low platinum (Pt) consumption is crucial for the cost reduction of energy devices, such as electrolyzers. Herein, nanoflower‐like carbon‐encapsulated CoNiPt alloy catalysts composition segregation are designed by pyrolyzing morphology‐controlled and Pt‐proportion‐tuned metal–organic frameworks (MOFs). The optimized containing 15% NFs (15%: Pt mass percentage, NFs: nanoflowers) exhibits outstanding HER performance a overpotential 25 mV at current density 10 mA cm −2 , far outperforming those commercial Pt/C (47 mV) most advanced catalysts. Such superior activity originates from integration Co‐O hybridization. hierarchical structure guarantees full exposure sites. Density functional theory calculations suggest that components not only promote water dissociation but also facilitate adsorption process, synergistically accelerating kinetics HER. In addition, volcanically distributed surface oxygen content, mainly in form Co 3d O 2p hybridization, which another reason enhanced activity. This work provides feasible insights into design cost‐effective coordinating kinetic sites adjusting appropriate content.

Language: Английский

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Mesoporous Pt@Pt-skin Pt3Ni core-shell framework nanowire electrocatalyst for efficient oxygen reduction

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

Published: March 18, 2023

The design of Pt-based nanoarchitectures with controllable compositions and morphologies is necessary to enhance their electrocatalytic activity. Herein, we report a rational synthesis anisotropic mesoporous Pt@Pt-skin Pt3Ni core-shell framework nanowires for high-efficient electrocatalysis. catalyst has uniform structure an ultrathin atomic-jagged Pt nanowire core Pt-skin shell, possessing high activity, stability utilisation efficiency. For the oxygen reduction reaction, demonstrated exceptional mass specific activities 6.69 A/mgpt 8.42 mA/cm2 (at 0.9 V versus reversible hydrogen electrode), exhibited negligible activity decay after 50,000 cycles. configuration combines advantages three-dimensional open mesopore molecular accessibility compressive surface strains, which results in more catalytically active sites weakened chemisorption oxygenated species, thus boosting its catalytic towards

Language: Английский

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Regulating Catalytic Properties and Thermal Stability of Pt and PtCo Intermetallic Fuel-Cell Catalysts via Strong Coupling Effects between Single-Metal Site-Rich Carbon and Pt

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(32), P. 17643 - 17655

Published: Aug. 4, 2023

Developing low platinum-group-metal (PGM) catalysts for the oxygen reduction reaction (ORR) in proton-exchange membrane fuel cells (PEMFCs) heavy-duty vehicles (HDVs) remains a great challenge due to highly demanded power density and long-term durability. This work explores possible synergistic effect between single Mn site-rich carbon (MnSA-NC) Pt nanoparticles, aiming improve intrinsic activity stability of PGM catalysts. Density functional theory (DFT) calculations predicted strong coupling MnN4 sites support, strengthening their interactions immobilize nanoparticles during ORR. The adjacent weaken adsorption at enhance activity. Well-dispersed (2.1 nm) ordered L12-Pt3Co (3.3 were retained on MnSA-NC support after indispensable high-temperature annealing up 800 °C, suggesting enhanced thermal stability. Both thoroughly studied electrode assemblies (MEAs), showing compelling performance Pt@MnSA-NC catalyst achieved mass (MA) 0.63 A mgPt–1 0.9 ViR-free maintained 78% its initial 30,000-cycle accelerated stress test (AST). L12-Pt3Co@MnSA-NC accomplished much higher MA 0.91 current 1.63 cm–2 0.7 V under traditional light-duty vehicle (LDV) H2–air conditions (150 kPaabs 0.10 mgPt cm–2). Furthermore, same an HDV MEA (250 0.20 cm–2) delivered 1.75 V, only losing 18% 90,000 cycles AST, demonstrating potential meet DOE targets.

Language: Английский

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Nanoscale Metal Particle Modified Single‐Atom Catalyst: Synthesis, Characterization, and Application

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(2)

Published: July 13, 2023

Single-atom catalysts (SACs) have attracted considerable attention in heterogeneous catalysis because of their well-defined active sites, maximum atomic utilization efficiency, and unique unsaturated coordinated structures. However, effectiveness is limited to reactions requiring sites containing multiple metal atoms. Furthermore, the loading amounts single-atom must be restricted prevent aggregation, which can adversely affect catalytic performance despite high activity individual The introduction nanoscale particles (NMPs) into SACs (NMP-SACs) has proven an efficient approach for improving performance. A comprehensive review urgently needed systematically introduce synthesis, characterization, application NMP-SACs mechanisms behind superior This first presents classifies different through NMPs enhance SACs. It then summarizes currently reported synthetic strategies state-of-the-art characterization techniques NMP-SACs. Moreover, electro/thermo/photocatalysis, reasons are discussed. Finally, challenges perspectives future design advanced addressed.

Language: Английский

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Fe–N–C Boosts the Stability of Supported Platinum Nanoparticles for Fuel Cells

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(44), P. 20372 - 20384

Published: Oct. 25, 2022

The poor durability of Pt-based nanoparticles dispersed on carbon black is the challenge for application long-life polymer electrolyte fuel cells. Recent work suggests that Fe- and N-codoped (Fe-N-C) might be a better support than conventional high-surface-area carbon. In this work, we find electrochemical surface area retention Pt/Fe-N-C much commercial Pt/C during potential cycling in both acidic basic media. situ inductively coupled plasma mass spectrometry studies indicate Pt dissolution rate 3 times smaller cycling. Density functional theory calculations further illustrate Fe-N-C substrate can provide strong stable to alleviate oxide formation by adjusting electronic structure. metal-substrate interaction, together with lower metal highly support, may reason significantly enhanced stability Pt/Fe-N-C. This finding highlights importance selection achieve more durable electrocatalyst

Language: Английский

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Synergistic Hybrid Electrocatalysts of Platinum Alloy and Single-Atom Platinum for an Efficient and Durable Oxygen Reduction Reaction

ACS Nano, Journal Year: 2022, Volume and Issue: 16(9), P. 14121 - 14133

Published: Aug. 26, 2022

Pt single-atom materials possess an ideal atom economy but suffer from limited intrinsic activity and side reaction of producing H2O2 in catalyzing the oxygen reduction (ORR); platinum alloys have higher weak stability. Here, we demonstrate that anchoring on Pt-decorated carbon (Pt-SAC) surmounts their inherent deficiencies, thereby enabling a complete four-electron ORR pathway catalysis with high efficiency durability. Pt3Co@Pt-SAC demonstrates exceptional mass specific activities 1 order magnitude than those commercial Pt/C. They are durable throughout 50000 cycles, showing only 10 mV decay half-wave potential. An situ Raman analysis theoretical calculations reveal Pt3Co core nanocrystals modulate electron structures adjacent single atoms to facilitate intermediate absorption for fast kinetics. The superior durability is attributed shielding effect Pt-SAC coating, which significantly mitigates dissolution cores. hybridizing strategy might promote development highly active catalysts.

Language: Английский

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