Pt‐Quantum‐Dot‐Modified Sulfur‐Doped NiFe Layered Double Hydroxide for High‐Current‐Density Alkaline Water Splitting at Industrial Temperature

Advanced Materials, Journal Year: 2023, Volume and Issue: unknown, P. 2208209 - 2208209

Published: Jan. 21, 2023

Suitable electrocatalysts for industrial water splitting can veritably promote practical hydrogen applications. Rational surface design is exceptionally significant to bridge the gap between fundamental science and expectation in splitting. Here, Pt-quantum-dot-modified sulfur-doped NiFe layered double hydroxides (Pt@S-NiFe LDHs) are designed with eximious catalytic activity toward evolution reaction (HER) under condition. Benefiting from enhanced binding energy, mass transfer, release, Pt@S-NiFe LDHs exhibit outstanding HER at high current densities. Notably, it obtains an impressively low overpotential of 71 mV long-term stability 200 h 100 mA cm-2 , exceeding commercial 40% Pt/C most reported Pt-based electrocatalysts. Its 2.7 times higher than that mV. Furthermore, temperature (65 °C), electrolyzer based on LDH needs just 1.62 V reach density superior one Pt/C//IrO2 . This work provides rational ideas develop exceptional performance high-temperature

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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Optimizing Pt-Based Alloy Electrocatalysts for Improved Hydrogen Evolution Performance in Alkaline Electrolytes: A Comprehensive Review

ACS Nano, Journal Year: 2023, Volume and Issue: 17(21), P. 20804 - 20824

Published: Nov. 3, 2023

The splitting of water through electrocatalysis offers a sustainable method for the production hydrogen. In alkaline electrolytes, lack protons forces dissociation to occur before hydrogen evolution reaction (HER). While pure Pt is gold standard electrocatalyst in acidic since 5d orbital nearly fully occupied, when it overlaps with molecular water, generates Pauli repulsion. As result, formation Pt–H* bond an environment difficult, which slows HER and negates benefits using catalyst. To overcome this limitation, can be alloyed transition metals, such as Fe, Co, Ni. This approach has potential not only enhance performance but also increase dispersion decrease its usage, thus overall improving catalyst's cost-effectiveness. excellent adsorption ability metals contributes generation proton-rich local near Pt-based alloy that promotes HER. Significant progress been achieved comprehending mechanism manipulation structure composition electrocatalysts based on alloy. objective review analyze condense latest developments It focuses modified alloys clarifies design principles catalytic catalysts from both experimental theoretical perspective. highlights some difficulties encountered during opportunities increasing performance. Finally, guidance development more efficient provided.

Language: Английский

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Optimizing Electrocatalytic Nitrogen Reduction via Interfacial Electric Field Modulation: Elevating d‐Band Center in WS₂‐WO₃ for Enhanced Intermediate Adsorption

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(29)

Published: May 25, 2023

Electrocatalytic nitrogen reduction reaction (ENRR) has emerged as a promising approach to synthesizing green ammonia under ambient conditions. Tungsten (W) is one of the most effective ENRR catalysts. In this reaction, protonation intermediates rate-determining step (RDS). Enhancing adsorption crucial increase intermediates, which can lead improved catalytic performance. Herein, we constructed strong interfacial electric field in WS2 -WO3 elevate d-band center W, thereby strengthening intermediates. Experimental results demonstrated that led significantly Specifically, exhibited high NH3 yield 62.38 μg h-1 mgcat-1 and promoted faraday efficiency (FE) 24.24 %. Furthermore, situ characterizations theoretical calculations showed upshifted W towards Fermi level, leading enhanced -NH2 -NH on catalyst surface. This resulted rate RDS. Overall, our study offers new insights into relationship between provides strategy enhance during process.

Language: Английский

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Surface engineering for stable electrocatalysis

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(5), P. 2693 - 2737

Published: Jan. 1, 2024

Unprecedented insights into electrochemical surface dynamics from operando studies inspire electronic and topographical strategies, paving the way for sustained electrocatalytic performance across HER, OER, ORR, CO 2 RR applications.

Language: Английский

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Mechanism of Particle-Mediated Inhibition of Demetalation for Single-Atom Catalytic Sites in Acidic Electrochemical Environments

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(28), P. 15528 - 15537

Published: July 10, 2023

Demetalation, caused by the electrochemical dissolution of metal atoms, poses a significant challenge to practical application single-atom catalytic sites (SACSs) in proton exchange membrane-based energy technologies. One promising approach inhibit SACS demetalation is use metallic particles interact with SACSs. However, mechanism underlying this stabilization remains unclear. In study, we propose and validate unified which can Fe Metal act as electron donors, decreasing oxidation state increasing density at FeN4 position, thereby strengthening Fe-N bond, inhibiting dissolution. Different types, forms, contents increase bond strength varying extents. A linear correlation between state, strength, amount supports mechanism. Our screening particle-assisted led 78% reduction dissolution, enabling continuous operation for up 430 h fuel cell. These findings contribute development stable SACSs applications.

Language: Английский

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Organocatalyst Supported by a Single‐Atom Support Accelerates both Electrodes used in the Chlor‐Alkali Industry via Modification of Non‐Covalent Interactions

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(8)

Published: Jan. 6, 2024

Consuming one of the largest amount electricity, chlor-alkali industry supplies basic chemicals for society, which mainly consists two reactions, hydrogen evolution (HER) and chlorine reaction (CER). Till now, state-of-the-art catalyst applied in this field is still dimensional stable anode (DSA), consumes a large noble metal Ru Ir. It thus necessary to develop new types catalysts. In study, an organocatalyst anchored on single-atom support (SAS) put forward. exhibits high catalytic efficiency towards both HER CER with overpotential 21 mV 20 at 10 mA cm

Language: Английский

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Pt Nanoparticle–Mn Single-Atom Pairs for Enhanced Oxygen Reduction

ACS Nano, Journal Year: 2024, Volume and Issue: 18(5), P. 4308 - 4319

Published: Jan. 23, 2024

The intrinsic roadblocks for designing promising Pt-based oxygen reduction reaction (ORR) catalysts emanate from the strong scaling relationship and activity–stability–cost trade-offs. Here, a carbon-supported Pt nanoparticle Mn single atom (PtNP–MnSA/C) as in situ constructed PtNP–MnSA pairs are demonstrated to be an efficient catalyst circumvent above seesaws with only ∼4 wt % loadings. Experimental theoretical investigations suggest that MnSA functions not "assist" sites cooperatively facilitate dissociation of O2 due electronic polarization, affording dissociative pathway reduced H2O2 production, but also structure "modulator" downshift d-band center sites, alleviating overbinding oxygen-containing intermediates. More importantly, serves "stabilizer" endow PtNP–MnSA/C excellent structural stability low Fenton-like reactivity, resisting fast demetalation metal sites. As result, PtNPs–MnSA/C shows ORR performance half-wave potential 0.93 V vs reversible hydrogen electrode high mass activity 1.77 A/mgPt at 0.9 acid media, which is 19 times higher than commercial Pt/C declines by 5% after 80,000 cycles. Specifically, reaches power density 1214 mW/cm2 2.87 A/cm2 H2–O2 fuel cell.

Language: Английский

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Efficient and durable seawater electrolysis with a V ₂ O ₃ -protected catalyst

Science Advances, Journal Year: 2024, Volume and Issue: 10(20)

Published: May 17, 2024

The ocean, a vast hydrogen reservoir, holds potential for sustainable energy and water development. Developing high-performance electrocatalysts production under harsh seawater conditions is challenging. Here, we propose incorporating protective V 2 O 3 layer to modulate the microcatalytic environment create in situ dual-active sites consisting of low-loaded Pt Ni N. This catalyst demonstrates an ultralow overpotential 80 mV at 500 mA cm −2 , mass activity 30.86 times higher than Pt-C maintains least hours seawater. Moreover, assembled anion exchange membrane electrolyzers (AEMWE) demonstrate superior durability even demanding industrial conditions. In localized pH analysis elucidates environmental regulation mechanism layer. Its role as Lewis acid enables sequestration excess OH − ions, mitigate Cl corrosion, alkaline earth salt precipitation. Our protection strategy by using presents promising cost-effective approach large-scale green production.

Language: Английский

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Construction of Surface Synergetic Oxygen Vacancies on CuMn₂O₄ Spinel for Enhancing NO Reduction with CO

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(5), P. 3028 - 3040

Published: Feb. 13, 2024

The effectiveness of surface synergetic oxygen vacancy (SSOV) on a catalyst has been proposed in the selective reduction NO to N2 by CO. In this work, we prepared fresh CuMn2O4 spinel using freeze-assisted sol–gel method, and then engineered SSOVs through CO pretreatment (CO–CuMn2O4) at 250 °C. catalytic performance CO–CuMn2O4 showed significant improvement, attributed presence SSOVs, comparison that sample. Additionally, our findings elucidated limited reactivity vacancies (SOVs) single metal oxide, emphasizing crucial role played SSOVs. Experimental results, including temperature-programmed desorption-mass spectrometry situ diffuse reflectance infrared Fourier transform spectroscopy, provided further insights suggesting facilitate formation N2O its subsequent decomposition into N2. Density functional theory calculations have unveiled pivotal SSOV stabilizing nitrogen atom derived from gaseous NO, facilitating + → N* CO2 reaction. Notably, energy barrier for process is only 0.54 eV, which rate-determining step stark contrast, reaction scarcely occurs SOVs CuO Mn2O3 surfaces. Furthermore, considerably lowers conversion N2, with minimal 0.12 eV. without assistance necessitates significantly higher 2.77 Extending investigation, CuFe2O4 observed similar SSOV-mediated effects Our research offers comprehensive understanding atomic-level SSOV, thereby offering valuable design efficient catalysts.

Language: Английский

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