Structure Engineering and Electronic Modulation of Transition Metal Interstitial Compounds for Electrocatalytic Water Splitting DOI
Yanqing Jiao, Haijing Yan, Chungui Tian

et al.

Accounts of Materials Research, Journal Year: 2022, Volume and Issue: 4(1), P. 42 - 56

Published: Dec. 1, 2022

ConspectusHydrogen is deemed as an ideal energy carrier because of its high density and clean nature. Water electrolysis fairly competitive for hydrogen production due to the conversion renewable electricity high-purity H2 with no carbon emission, in comparison traditional industrial technology. However, large-scale application hampered by cost partially from use noble metal-based catalysts promote kinetics oxygen evolution reactions. Developing cost-efficient transition electrocatalysts, therefore, a hopeful prospect, they can provide d-orbital lone-pair electrons or empty d-orbitals adsorbing different intermediates (such H*, OH*, O*, OOH*). As compared metals their oxides, metal interstitial compounds (TMICs) formed inserting C, N, P atoms into sites parent hold distinct advantages Pt-like electronic structure, conductivity, superior chemical stability over wide pH range, beneficial overcoming consumption faced alkaline water intractable issue acid electrolysis. Nevertheless, major drawbacks are large size, density, sluggish ionic kinetics, resulting ordinary electrochemical activity low mass efficiency. Electrocatalytic performance dominated intrinsic activity, number accessible active sites, capacity charge transfer. Engineering micronano structure (small-size particles, porous ultrathin nanosheet) expose more catalytical facilitate transport gas diffusion. Meanwhile, modulating optimize adsorption boost activity. Apparently, synergistic modulation TMICs expected achieve multiobjective optimization targeting highly effective catalysts.In this Account, we summarize our recent efforts designed synthesis engineering utilizing polyoxometalates (POMs) precursors associated strategies advance electrocatalytic toward HER OER. We start brief summary OER mechanisms, which play crucial roles elaborate design relevant electrocatalysts. The disadvantages pointed out, apart opportunities offered POMs constructing novel component, interface structure. Several efficient enhancement proposed including reducing size heterojunctions interfaces, doping heteroatoms regulate binding intermediates, creating pores accelerate transfer, etc. Accordingly, controllable well-defined highlighted, positive role tailoring on enhancing catalytic efficiency confirmed. Furthermore, paired electrocatalysis using species produce value-added chemicals reduce consumption. Finally, remaining challenges, opportunities, future development directions TMICs-based materials discussed.

Language: Английский

Modulating the Electronic Structure of Cobalt‐Vanadium Bimetal Catalysts for High‐Stable Anion Exchange Membrane Water Electrolyzer DOI

Zhijian Liang,

Di Shen, Wei Yao

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(41)

Published: Aug. 15, 2024

Abstract Modulating the electronic structure of catalysts to effectively couple hydrogen evolution reaction (HER) and oxygen (OER) is essential for developing high‐efficiency anion exchange membrane water electrolyzer (AEMWE). Herein, a coral‐like nanoarray composed nanosheets through synergistic layering effect cobalt 1D guiding vanadium synthesized, which promotes extensive contact between active sites electrolyte. The HER OER activities can be enhanced by modulating nitridation phosphorization, respectively, enhancing strength metal‐H bond optimize adsorption facilitating proton transfer improve transformation oxygen‐containing intermediates. Resultantly, AEMWE achieves current density 500 mA cm –2 at 1.76 V 1000 h in 1.0 M KOH 70 °C. energy consumption 4.21 kWh Nm –3 with producing cost $0.93 per kg H 2 . Operando synchrotron radiation Bode phase angle analyses reveal that during high‐energy consumed OER, dissolution species transforms distorted Co−O octahedral into regular structures, accompanied shortening Co−Co length. This structural facilitates formation intermediates, thus accelerating kinetics.

Language: Английский

Citations

28

An oxygen-coordinated cobalt single-atom electrocatalyst boosting urea and urea peroxide production DOI
Shengbo Zhang, Jin Meng, Hui Xu

et al.

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(5), P. 1950 - 1960

Published: Jan. 1, 2024

An oxygen-coordinated cobalt single-atom catalyst was successfully fabricated, exhibiting exceptional electrocatalytic activity toward urea and H 2 O production. Subsequently, the value-added peroxide efficiently synthesized.

Language: Английский

Citations

25

Tailoring First Coordination Sphere of Dual‐Metal Atom Sites Boosts Oxygen Reduction and Evolution Activities DOI
Zhe Wang,

Ruojie Xu,

Qitong Ye

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(28)

Published: Feb. 24, 2024

Abstract It is important to tune the coordination configuration of dual‐atom catalyst (DAC), especially in first sphere, render high intrinsic catalytic activities for oxygen reduction/evolution reactions (ORR/OER). Herein, a type atomically dispersed and boron‐coordinated DAC structure, namely, FeN 4 B‐NiN B dual sites, reported. In this incorporation boron into sphere /NiN atomic sites regulates its geometry electronic structure by forming “Fe‐B‐N” “Ni‐B‐N” bridges. The exhibits much enhanced ORR OER property compared ‐NiN counterparts. Density functional theory calculations reveal that boron‐induced charge transfer asymmetric distributions central Fe/Ni atoms optimize adsorption desorption behavior ORR/OER intermediates reduce activation energy potential‐determining step. Zinc‐air batteries employing cathode exhibit maximum power density (236.9 mW cm −2 ) stable cyclability up 1100 h. result illustrates pivotal role first‐coordination DACs tuning electrochemical conversion storage activities.

Language: Английский

Citations

24

Selective oxygen reduction reaction: mechanism understanding, catalyst design and practical application DOI Creative Commons
Shilong Li, Lei Shi, Yingjie Guo

et al.

Chemical Science, Journal Year: 2024, Volume and Issue: 15(29), P. 11188 - 11228

Published: Jan. 1, 2024

The oxygen reduction reaction (ORR) is a key component for many clean energy technologies and other industrial processes. However, the low selectivity sluggish kinetics of ORR catalysts have hampered conversion efficiency real application these new mentioned before. Recently, tremendous efforts been made in mechanism understanding, electrocatalyst development system design. Here, comprehensive critical review provided to present recent advances field electrocatalytic ORR. two-electron four-electron transfer catalytic mechanisms evaluation parameters are discussed first. Then, up-to-date synthetic strategies

Language: Английский

Citations

22

Structure Engineering and Electronic Modulation of Transition Metal Interstitial Compounds for Electrocatalytic Water Splitting DOI
Yanqing Jiao, Haijing Yan, Chungui Tian

et al.

Accounts of Materials Research, Journal Year: 2022, Volume and Issue: 4(1), P. 42 - 56

Published: Dec. 1, 2022

ConspectusHydrogen is deemed as an ideal energy carrier because of its high density and clean nature. Water electrolysis fairly competitive for hydrogen production due to the conversion renewable electricity high-purity H2 with no carbon emission, in comparison traditional industrial technology. However, large-scale application hampered by cost partially from use noble metal-based catalysts promote kinetics oxygen evolution reactions. Developing cost-efficient transition electrocatalysts, therefore, a hopeful prospect, they can provide d-orbital lone-pair electrons or empty d-orbitals adsorbing different intermediates (such H*, OH*, O*, OOH*). As compared metals their oxides, metal interstitial compounds (TMICs) formed inserting C, N, P atoms into sites parent hold distinct advantages Pt-like electronic structure, conductivity, superior chemical stability over wide pH range, beneficial overcoming consumption faced alkaline water intractable issue acid electrolysis. Nevertheless, major drawbacks are large size, density, sluggish ionic kinetics, resulting ordinary electrochemical activity low mass efficiency. Electrocatalytic performance dominated intrinsic activity, number accessible active sites, capacity charge transfer. Engineering micronano structure (small-size particles, porous ultrathin nanosheet) expose more catalytical facilitate transport gas diffusion. Meanwhile, modulating optimize adsorption boost activity. Apparently, synergistic modulation TMICs expected achieve multiobjective optimization targeting highly effective catalysts.In this Account, we summarize our recent efforts designed synthesis engineering utilizing polyoxometalates (POMs) precursors associated strategies advance electrocatalytic toward HER OER. We start brief summary OER mechanisms, which play crucial roles elaborate design relevant electrocatalysts. The disadvantages pointed out, apart opportunities offered POMs constructing novel component, interface structure. Several efficient enhancement proposed including reducing size heterojunctions interfaces, doping heteroatoms regulate binding intermediates, creating pores accelerate transfer, etc. Accordingly, controllable well-defined highlighted, positive role tailoring on enhancing catalytic efficiency confirmed. Furthermore, paired electrocatalysis using species produce value-added chemicals reduce consumption. Finally, remaining challenges, opportunities, future development directions TMICs-based materials discussed.

Language: Английский

Citations

53