Conductive Covalent Organic Frameworks of Polymetallophthalocyanines as a Tunable Platform for Electrocatalysis DOI
Yi Zhang, Xiyuan Zhang, Long Jiao

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(44), P. 24230 - 24239

Published: Oct. 27, 2023

Developing an electrocatalyst platform that can control the interplay among activity, selectivity, and stability at atomic precision remains a grand challenge. Here, we have synthesized highly crystalline polymetallophthalocyanines (pMPcs, M = Fe, Co, Ni, Cu) through annulation of tetracyanobenzene in presence transition metals. The conjugated, conductive, stable backbones with precisely installed metal sites render pMPcs unique electrochemical catalysis, where tunability emerges from long-range interactions. construction pCoNiPc Co Ni dual-site integrates advantageous features pCoPc pNiPc electrocatalytic CO2 reduction electronic communication unprecedented long separation ≥14 chemical bonds. This integration provides excellent activity (current density, j -16.0 -100 mA cm-2 H-type flow cell, respectively), selectivity (CO Faraday efficiency, FECO 94%), (>10 h), making it one best-performing reticular materials.

Language: Английский

Ligand Modulation of Active Sites to Promote Electrocatalytic Oxygen Evolution DOI

Wenzhong Huang,

Jiantao Li, Xiaobin Liao

et al.

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(18)

Published: March 12, 2022

Rationally designed catalysts hold the key to address sluggish kinetics of oxygen evolution reaction (OER). However, engineering active sites such still faces grand challenges. This study proposes a feasible ligand modulation strategy boost OER catalytic activity cobalt-iron oxyhydroxide ((Fe,Co)OOH). The 2-methylimidazole (MI) coordination on (Fe,Co)OOH reduces orbital overlap between Fe/Co 3d and O 2p, which weakens adsorption oxygen-containing intermediates thus facilitates unfavorable O2 desorption. As result, MI modulated achieves an excellent performance with low overpotentials (230/290 mV at 10/100 mA cm-2 ) durability (>155 h). provides novel for design catalysts.

Language: Английский

Citations

185

Seven steps to reliable cyclic voltammetry measurements for the determination of double layer capacitance DOI Creative Commons
Dulce M. Morales, Marcel Risch

Journal of Physics Energy, Journal Year: 2021, Volume and Issue: 3(3), P. 034013 - 034013

Published: March 12, 2021

Abstract Discovery of electrocatalytic materials for high-performance energy conversion and storage applications relies on the adequate characterization their intrinsic activity, which is currently hindered by dearth a protocol consistent precise determination double layer capacitance ( C DL ). Herein, we propose seven-step method that aims to determine reliably scan rate-dependent cyclic voltammetry considering aspects strongly influence outcome analysis, including (a) selection suitable measuring window, (b) uncompensated resistance, (c) optimization settings, (d) data acquisition, (e) (f) extraction desired information, (g) validation results. To illustrate proposed method, two systems were studied: resistor–capacitor electric circuit, glassy carbon disk in an electrochemical cell. With these studies, it demonstrated when any mentioned steps procedure are neglected, substantial deviations results observed with misestimations as large 61% case investigated system. Moreover, allometric regression more model than linear both ideal non-ideal investigated. We stress importance assessing accuracy not only highly specialized methods, but also those well-known commonly used voltammetric methods. The herein limited , can be effectively applied other analysis deliver quantitative via crucial study kinetic diffusion phenomena systems.

Language: Английский

Citations

146

Recent advances in interface engineering strategy for highly‐efficient electrocatalytic water splitting DOI Creative Commons
Yunmei Du, Bin Li, Guangrui Xu

et al.

InfoMat, Journal Year: 2022, Volume and Issue: 5(1)

Published: Oct. 13, 2022

Abstract The hydrogen energy generated by the electrocatalytic water splitting reaction has been established as a renewable and clean carrier with ultra‐high density, which can well make up for shortcomings of conventional sources, such geographical limitations, climatic dependence, wastage. Notably, introduction electrocatalysts enhance efficiency process to generate hydrogen. Particularly, heterostructure constructed coupling multiple components (or phases) have emerged most promising option due well‐known electronic synergistic effects. existing reviews on interface engineering electrocatalyst design mostly focus relationship between heterostructures specific reactions. However, comprehensive overview integration model building, directional synthesis, mechanism rarely reported. To this end, in review, development catalysts is systematically introduced from perspective classification, growth regulation performance based interfacial microenvironment (bonding, configuration, lattice strain, etc.), thereby offering useful insights construction models. Besides, combined current applications strategies, challenges future are discussed relevant solutions proposed. Overall, review serve theoretical reference mechanism, further promote production technologies low consumption high yield. image

Language: Английский

Citations

138

Strain Relaxation in Metal Alloy Catalysts Steers the Product Selectivity of Electrocatalytic CO2 Reduction DOI

Jican Hao,

Zechao Zhuang, Jiace Hao

et al.

ACS Nano, Journal Year: 2022, Volume and Issue: 16(2), P. 3251 - 3263

Published: Jan. 28, 2022

Strain engineering in bimetallic alloy structures is of great interest electrochemical CO2 reduction reactions (CO2RR), which it simultaneously improves electrocatalytic activity and product selectivity by optimizing the binding properties intermediates. However, a reliable synthetic strategy systematic understanding strain effects CO2RR are still lacking. Herein, we report relaxation used to determine lattice strains bimetal MNi alloys (M = Pd, Ag, Au) realize an outstanding CO2-to-CO Faradaic efficiency 96.6% show durability toward Zn-CO2 battery. Molecular dynamics (MD) simulations predict that strained PdNi (s-PdNi) correlated with increases synthesis temperature, high temperature activation energy drives complete atomic mixing multiple metal atoms allow for regulation strains. Density functional theory (DFT) calculations reveal effectively formation energies *COOH *CO intermediates on s-PdNi surfaces, as also verified situ spectroscopic investigations. This approach provides promising catalyst design, enabling independent optimization reaction improve catalytic simultaneously.

Language: Английский

Citations

137

Silver nanomaterials: synthesis and (electro/photo) catalytic applications DOI
Rakesh Kumar Sharma, Sneha Yadav, Sriparna Dutta

et al.

Chemical Society Reviews, Journal Year: 2021, Volume and Issue: 50(20), P. 11293 - 11380

Published: Jan. 1, 2021

In view of their unique characteristics and properties, silver nanomaterials (Ag NMs) have been used not only in the field nanomedicine but also for diverse advanced catalytic technologies. this comprehensive review, light is shed on general synthetic approaches encompassing chemical reduction, sonochemical, microwave, thermal treatment among preparative methods syntheses Ag-based NMs applications. Additionally, some latest innovative such as continuous flow integrated with MW other benign emphasized that ultimately pave way sustainability. Moreover, potential applications emerging Ag NMs, including sub single atoms, liquid-phase catalysis, photocatalysis, electrocatalysis well a positive role reactions are meticulously summarized. The scientific interest synthesis lies benefits activity, selectivity, stability, recovery. Therefore, rise journey NM-based catalysts will inspire new generation chemists to tailor design robust can effectively tackle major environmental challenges help replace noble metals This overview concludes by providing future perspectives research into arena photocatalysis.

Language: Английский

Citations

134

Interatomic Electronegativity Offset Dictates Selectivity When Catalyzing the CO2 Reduction Reaction DOI

Jican Hao,

Zechao Zhuang, Jiace Hao

et al.

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(26)

Published: June 1, 2022

Abstract Achieving efficient efficiency and selectivity for the electroreduction of CO 2 to value‐added feedstocks has been challenging, due thermodynamic stability molecules competing hydrogen evolution reaction. Herein, a dual‐single‐atom catalyst consisting atomically dispersed CuN 4 NiN bimetal sites is synthesized with electrospun carbon nanofibers (CuNi‐DSA/CNFs). Theoretical experimental studies reveal strong electron interactions induced by electronegativity offset between Cu Ni atoms. The delicately averaged compensated electronic structures result in an effect that optimizes adsorption strength *COOH intermediate boosts reduction reaction (CO RR) kinetics, notably promoting intrinsic activity catalyst. CuNi‐DSA/CNFs exhibits outstanding FE 99.6% across broad potential window −0.78– −1.18 V (vs reversible electrode), high turnover frequency 2870 h –1 , excellent durability (25 h). Furthermore, aqueous Zn‐CO battery power conversion constructed. This atomic‐level dual‐atom provides appealing direction develop advanced electrocatalysts RR.

Language: Английский

Citations

134

Aluminum-air batteries: A review of alloys, electrolytes and design DOI
Robert Buckingham, Tristan Asset, Plamen Atanassov

et al.

Journal of Power Sources, Journal Year: 2021, Volume and Issue: 498, P. 229762 - 229762

Published: April 30, 2021

Language: Английский

Citations

132

Bi2O3/BiO2 Nanoheterojunction for Highly Efficient Electrocatalytic CO2 Reduction to Formate DOI
Xuezhen Feng, Haiyuan Zou, Renji Zheng

et al.

Nano Letters, Journal Year: 2022, Volume and Issue: 22(4), P. 1656 - 1664

Published: Feb. 4, 2022

Heterostructure engineering plays a vital role in regulating the material interface, thus boosting electron transportation pathway advanced catalysis. Herein, novel Bi2O3/BiO2 heterojunction catalyst was synthesized via molten alkali-assisted dealumination strategy and exhibited rich structural dynamics for an electrocatalytic CO2 reduction reaction (ECO2RR). By coupling situ X-ray diffraction Raman spectroscopy measurements, we found that as-synthesized heterostructure can be transformed into Bi/BiO2 Mott–Schottky heterostructure, leading to enhanced adsorption performance *OCHO intermediates. Consequently, high selectivity toward formate larger than 95% rendered wide potential window along with optimum partial current density of −111.42 mA cm–2 benchmarked state-of-the-art Bi-based ECO2RR catalysts. This work reports construction fruitful dynamic insights electrocatalyst ECO2RR, which paves way rational design efficient electrocatalysts beyond.

Language: Английский

Citations

130

Noble-metal-based high-entropy-alloy nanoparticles for electrocatalysis DOI
Xian‐Feng Huang, Guangxing Yang, Shuang Li

et al.

Journal of Energy Chemistry, Journal Year: 2021, Volume and Issue: 68, P. 721 - 751

Published: Dec. 23, 2021

Language: Английский

Citations

118

Crossing the Valley of Death: From Fundamental to Applied Research in Electrolysis DOI Creative Commons
Daniel Siegmund, Sebastian Metz,

Volker Peinecke

et al.

JACS Au, Journal Year: 2021, Volume and Issue: 1(5), P. 527 - 535

Published: April 12, 2021

The growing societal and political focus on the use of environmentally friendly technologies has led to an ever-increasing interest in electrolysis scientific communities. This development is reflected by plethora candidate catalysts for hydrogen oxygen evolution reactions, as well CO2 reduction reaction, reported literature. However, almost none them entered stage application yet. Likewise, reports process engineering inadequately address utilization these catalysts, electrode cell concepts, that might be suitable market. Evidently, a closer collaboration between chemists engineers from industry academia desirable speed up disruptive technologies. Herein, we elucidate critical parameters highlight necessary aspects accelerate industrially relevant capable fulfilling forthcoming challenges related energy conversion storage. aim this Perspective, composed industrial academic partners, critically question current undertakings encourage researchers strike interdisciplinary research pathways.

Language: Английский

Citations

116