Constructing molecule-metal relay catalysis over heterophase metallene for high-performance rechargeable zinc-nitrate/ethanol batteries

Proceedings of the National Academy of Sciences, Год журнала: 2023, Номер 120(50)

Опубликована: Дек. 8, 2023

Zinc-nitrate batteries can integrate energy supply, ammonia electrosynthesis, and sewage disposal into one electrochemical device. However, current zinc-nitrate still severely suffer from the limited density poor rechargeability. Here, we report synthesis of tetraphenylporphyrin (tpp)-modified heterophase (amorphous/crystalline) rhodium-copper alloy metallenes (RhCu M-tpp). Using RhCu M-tpp as a bifunctional catalyst for nitrate reduction reaction (NO

Язык: Английский

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Ultrafine Core@Shell Cu₁Au₁@Cu₁Pd₃ Nanodots Synergized with 3D Porous N-Doped Graphene Nanosheets as a High-Performance Multifunctional Electrocatalyst

ACS Nano, Год журнала: 2023, Номер 17(3), С. 2992 - 3006

Опубликована: Янв. 27, 2023

Rationally combining designed supports and metal-based nanomaterials is effective to synergize their respective physicochemical electrochemical properties for developing highly active stable/durable electrocatalysts. Accordingly, in this work, sub-5 nm monodispersed nanodots (NDs) with the special nanostructure of an ultrafine Cu1Au1 core a 2-3-atomic-layer Cu1Pd3 shell are synthesized by facile solvothermal method, which further evenly firmly anchored onto 3D porous N-doped graphene nanosheets (NGS) via simple annealing (A) process. The as-obtained Cu1Au1@Cu1Pd3 NDs/NGS-A exhibits exceptional electrocatalytic activity noble-metal utilization toward alkaline oxygen reduction, methanol oxidation, ethanol oxidation reactions, showing dozens-fold enhancements compared commercial Pd/C Pt/C. Besides, it also has excellent long-term stability durability. Advanced comprehensive experimental theoretical analyses unveil synthetic mechanism core@shell reveal origins significantly enhanced performance: (1) prominent structural NGS, (2) ultrasmall size as well uniform morphology NDs-A, (3) Cu-Au-Pd alloy subnanometer shell, (4) strong metal-support interaction. This work not only develops method fabricating ultrafine-core@ultrathin-shell but proposes practical design paradigm comprehensively rationally considering both realizing high-performance multifunctional electrocatalysts, can be expanded other energy-conversion or environmental (electro)catalytic applications.

Язык: Английский

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RhCuBi Trimetallenes with Composition Segregation Coupled Crystalline‐Amorphous Heterostructure Toward Ethanol Electrooxidation

Advanced Energy Materials, Год журнала: 2024, Номер 14(21)

Опубликована: Фев. 19, 2024

Abstract The inefficiency of Pt and Pd benchmark catalysts in achieving complete ethanol oxidation, coupled with their inherent susceptibility to poisoning, poses a significant obstacle the advancement direct fuel cells. In this study, development self‐supported ultrathin RhCuBi trimetallenes, demonstrating exceptional performance electrooxidation through segregation interface engineering is presented. distinctive RhBi‐rich crystalline/RhCu‐rich amorphous heterostructure trimetallenes creates wealth highly active interfacial sites for oxidation reaction (EOR). This results an impressive 43.3% Faradaic efficiency C1 pathway peak mass activity 1.11 A mg Rh −1 at 0.68 V versus reversible hydrogen electrode. Moreover, retain 60% initial after 8.5 h constant potential electrolysis, outperforming commercial (<3%). In/ex situ infrared spectroscopy directly reveals generated products key CH 3 CO* intermediates EOR on trimetallenes. Theoretical calculations confirm that RhBi alloy, particularly lattice‐stretched crystalline/amorphous sites, facilitates adsorption/activation dehydrogenation toward EOR. breakthrough offers promising prospects enhancing stability cell applications.

Язык: Английский

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Phosphorus doped PdMo bimetallene as a superior bifunctional fuel cell electrocatalyst

Chemical Engineering Journal, Год журнала: 2024, Номер 486, С. 150258 - 150258

Опубликована: Март 8, 2024

Язык: Английский

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Regulating the Electrochemical Nitrate Reduction Performance with Controllable Distribution of Unconventional Phase Copper on Alloy Nanostructures

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Сен. 6, 2024

Abstract Electrochemical nitrate reduction reaction (NO 3 RR) is emerging as a promising strategy for removal and ammonia (NH ) production using renewable electricity. Although great progresses have been achieved, the crystal phase effect of electrocatalysts on NO RR remains rarely explored. Here, epitaxial growth unconventional 2H Cu hexagonal close‐packed ( hcp IrNi template, resulting in formation three IrNiCu@Cu nanostructures, reported. IrNiCu@Cu‐20 shows superior catalytic performance, with NH Faradaic efficiency (FE) 86% at −0.1 (vs reversible hydrogen electrode [RHE]) yield rate 687.3 mmol g −1 h , far better than common face‐centered cubic Cu. In sharp contrast, IrNiCu@Cu‐30 IrNiCu@Cu‐50 covered by shell display high selectivity toward nitrite 2 − ), FE above 60% 0.1 RHE). Theoretical calculations demonstrated that has optimal electronic structures due to highest d‐band center strongest trend lowest energy barriers. The electroactivity originates from abundant low coordination sites surface, which guarantees fast electron transfer accelerate intermediate conversions. This work provides feasible tactic regulate product distribution engineering electrocatalysts.

Язык: Английский

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Intermetallic Synergy in PdCuCo Catalysts Boosts C─C Bond Cleavage of Polyalcohol Electrooxidation

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Фев. 9, 2025

Abstract Multi‐metallic catalysts with specific structures play a crucial role in enhancing the selectivity and activity of chemical reactions. However, challenges such as unfavorable alcohol adsorption on catalysts, CO poisoning, high free energy barriers during oxidation processes pose significant obstacles to catalysts' ability cleave C─C bonds for complete oxidation. Here, series PdCuCo metalene electrocatalysts is reported, wherein varying intermetallic interactions among Pd, Cu, Co effectively modulate pathway. Notably, catalyst Pd 0.15 Cu 0.35 2 , synthesized by galvanic replacement metallic surface, delivers remarkably electrocatalytic ethylene glycol glycerol alkaline electrolytes (9.7 10.9 A mg −1 respectively), both which are much better than reported broadly applicable various alcohols. High performance assigned structural advantages material synergistic effects multiple metals. This synergy not merely enhances surface electronics, fostering creation exclusive active sites, but also facilitates oxidative cleavage stable bond efficient

Язык: Английский

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Electrocatalytic Reduction of Carbon Dioxide to High-Value Multicarbon Products with Metal–Organic Frameworks and Their Derived Materials

ACS Materials Letters, Год журнала: 2022, Номер 4(11), С. 2058 - 2079

Опубликована: Сен. 26, 2022

The electrocatalytic carbon dioxide reduction reaction (CO2RR) holds great potential in promoting neutral through effectively converting CO2 molecules to useful chemicals and fuels. high-efficiency electrochemical conversion of single-carbon products has been well realized, while more efforts are needed for the generation high-value multicarbon products. Metal–organic frameworks (MOFs), featuring porous structures, high chemical tunability, ultralarge surface area, have attracted increasing attention CO2RR. Herein, we review recent progress CO2RR on MOF-based materials toward First, structure MOFs is briefly introduced. Then, performance corresponding catalytic mechanism pristine (classified according kind organic ligands/linkers) MOF-derived (including metal nanomaterials, single-atom catalysts nanocomposites) product systematically discussed. Finally, critical challenges opportunities highlighted inspire rational design targeted synthesis advanced high-performance

Язык: Английский

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Electro‐Synthesis of Organic Compounds with Heterogeneous Catalysis

Advanced Science, Год журнала: 2022, Номер 10(1)

Опубликована: Ноя. 18, 2022

Electro-organic synthesis has attracted a lot of attention in pharmaceutical science, medicinal chemistry, and future industrial applications energy storage conversion. To date, there not been detailed review on electro-organic with the strategy heterogeneous catalysis. In this review, most recent advances synthesizing value-added chemicals by catalysis are summarized. An overview electrocatalytic oxidation reduction processes as well paired electrocatalysis is provided, anodic alcohols (monohydric polyhydric), aldehydes, amines discussed. This also provides in-depth insight into cathodic carboxylates, carbon dioxide, CC, C≡C, reductive coupling reactions. Moreover, electro-synthesis methods, including parallel paired, sequential divergent convergent electrolysis, Additionally, strategies developed to achieve high electrosynthesis efficiency associated challenges addressed. It believed that promising direction organic electrochemistry, offering numerous opportunities develop new reaction methods.

Язык: Английский

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Interfacial electric field effect on electrochemical carbon dioxide reduction reaction

Chem Catalysis, Год журнала: 2022, Номер 2(9), С. 2229 - 2252

Опубликована: Авг. 26, 2022

Язык: Английский

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Rapid detection of low concentration H2 using Au@Pd/SnO2 nanocomposites

Sensors and Actuators B Chemical, Год журнала: 2022, Номер 366, С. 131971 - 131971

Опубликована: Апрель 28, 2022

Язык: Английский

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