Molecule-Enhanced Electrocatalysis of Sustainable Oxygen Evolution Using Organoselenium Functionalized Metal–Organic Nanosheets DOI
Liming Cao,

Chang-Guo Hu,

Haihong Li

et al.

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 145(2), P. 1144 - 1154

Published: Dec. 20, 2022

Remolding the reactivity of metal active sites is critical to facilitate renewable electricity-powered water electrolysis. Doping heteroatoms, such as Se, into a crystal lattice has been considered an effective approach, yet usually suffers from loss functional heteroatoms during harsh electrocatalytic conditions, thus leading gradual inactivation catalysts. Here, we report new heteroatom-containing molecule-enhanced strategy toward sustainable oxygen evolution improvement. An organoselenium ligand, bis(3,5-dimethyl-1H-pyrazol-4-yl)selenide containing robust C–Se–C covalent bonds equipped in precatalyst ultrathin metal–organic nanosheets Co-SeMON, revealed significantly enhance catalytic mass activity cobalt site by 25 times, well extend catalyst operation time alkaline conditions 1 or 2 orders magnitude compared with these reported selenides. A combination various situ/ex situ spectroscopic techniques, ab initio molecular dynamics, and density theory calculations unveiled intensified mechanism, which nonclassical bonding Se O-containing intermediates endows adsorption-energy regulation beyond conventional scaling relationship. Our results showcase great potential catalysts for highly efficient economical oxidation.

Language: Английский

Current Progress in 2D Metal–Organic Frameworks for Electrocatalysis DOI Creative Commons
Usman Khan,

Adeela Nairan,

Junkuo Gao

et al.

Small Structures, Journal Year: 2022, Volume and Issue: 4(6)

Published: Sept. 16, 2022

The 2D nanosheets of metal–organic frameworks (MOFs) have recently emerged as a promising material that makes them valuable in widespread electrocatalytic fields due to their atomic‐level thickness, abundant active sites, and large surface area. Efficient electrocatalysts for hydrogen evolution reaction (HER), oxygen (OER), overall water splitting are highly desired with low overpotentials promote the industrial applications energy conversion devices. MOF nanostructures provide long‐term stability high electrical conductivity enhance catalyst activity durability. This review briefly summarizes synthesis HER/OER/water splitting. More attention is focused on synthetic strategies derivatives. catalytic performance superior properties these materials highlighted. outperformance originates from rational design, myriad thickness. current future challenges this field scientific perspectives overcome It suggested construction can develop state‐of‐the‐art electrocatalyst environmental division.

Language: Английский

Citations

174
Metal–Organic Frameworks as Electrocatalysts DOI
Yong Peng,

Soheila Sanati,

Ali Morsali

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(9)

Published: Dec. 5, 2022

Abstract Transition metal complexes are well‐known homogeneous electrocatalysts. In this regard, metal–organic frameworks (MOFs) can be considered as an ensemble of transition ordered in a periodic arrangement. addition, MOFs have several additional positive structural features that make them suitable for electrocatalysis, including large surface area, high porosity, and content accessible with exchangeable coordination positions. The present review describes the current state use electrocatalysts, both host electroactive guests their direct electrocatalytic activity, particularly case bimetallic MOFs. field MOF‐derived materials is purposely not covered, focusing on or its composites Special attention has been paid to strategies overcome poor electrical conductivity limited stability.

Language: Английский

Citations

111
Design of modified MOFs electrocatalysts for water splitting: High current density operation and long-term stability DOI
Yangping Zhang, Xiangjun Zheng, Xingmei Guo

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 336, P. 122891 - 122891

Published: May 18, 2023

Language: Английский

Citations

107
2D Metal–Organic Frameworks as Competent Electrocatalysts for Water Splitting DOI

Chaopeng Wang,

Yuxuan Lin, Lei Cui

et al.

Small, Journal Year: 2023, Volume and Issue: 19(15)

Published: Jan. 5, 2023

Hydrogen, a clean and flexible energy carrier, can be efficiently produced by electrocatalytic water splitting. To accelerate the sluggish hydrogen evolution reaction oxygen kinetics in splitting process, highly active electrocatalysts are essential for lowering barriers, thereby improving efficiency of overall Combining distinctive advantages metal-organic frameworks (MOFs) with physicochemical properties 2D materials such as large surface area, tunable structure, accessible sites, enhanced conductivity, MOFs have attracted intensive attention field electrocatalysis. Different strategies, conductivities MOFs, reducing thicknesses MOF nanosheets, integrating conductive particles or substrates, developed to promote catalytic performances pristine MOFs. This review summarizes recent advances MOF-based electrolysis. In particular, their intrinsic detailly analyzed reveal important roles inherent centers, other situ generated phases from responsible reactions. Finally, challenges development prospects future applications discussed.

Language: Английский

Citations

87
Flexible Cuprous Triazolate Frameworks as Highly Stable and Efficient Electrocatalysts for CO2 Reduction with Tunable C2H4/CH4 Selectivity DOI

Lin‐Ling Zhuo,

Pin Chen, Kai Zheng

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(28)

Published: May 5, 2022

Cu-based metal-organic frameworks have attracted much attention for electrocatalytic CO2 reduction, but they are generally instable and difficult to control the product selectivity. We report flexible Cu(I) triazolate as efficient, stable, tunable electrocatalysts reduction C2 H4 /CH4 . By changing size of ligand side groups, selectivity ratio can be gradually tuned inversed from 11.8 : 1 2.6, giving , CH4 hydrocarbon selectivities up 51 %, 56 77 respectively. After long-term electrocatalysis, retain structures/morphologies without formation inorganic species. Computational simulations showed that coordination geometry changed triangular tetrahedral bind reaction intermediates, two adjacent cooperated C-C coupling form Importantly, groups controlled catalyst flexibility by steric hindrance mechanism, pathway is more sensitive than one.

Language: Английский

Citations

85
The emerging aqueous zinc-organic battery DOI
Heng‐guo Wang, Qiong Wu, Linqi Cheng

et al.

Coordination Chemistry Reviews, Journal Year: 2022, Volume and Issue: 472, P. 214772 - 214772

Published: Aug. 19, 2022

Language: Английский

Citations

81
Rational design and synthesis of two-dimensional conjugated metal-organic polymers for electrocatalysis applications DOI Creative Commons
Liu Lin, Qiu Zhang,

Youxuan Ni

et al.

Chem, Journal Year: 2022, Volume and Issue: 8(7), P. 1822 - 1854

Published: June 11, 2022

Language: Английский

Citations

80
Conjugated Coordination Polymer as a New Platform for Efficient and Selective Electroreduction of Nitrate into Ammonia DOI
Yizhe Zhang, Hui Zheng, Kangjie Zhou

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(10)

Published: Jan. 18, 2023

Electroreduction of nitrate into ammonia (NRA) provides a sustainable route to convert the widespread pollutants high-value-added products under ambient conditions, which unfortunately suffers from unsatisfactory selectivity due competitive hydrogen evolution reaction (HER). Previous strategies modifying metal sites catalysts often met dilemma for simultaneously promoting activity and toward NRA. Here, general strategy is reported enable an efficient selective NRA process through coordination modulation single-atom tailor local proton concentration at catalyst surface. By contrast, two analogous Ni-single-atom enriched conjugated polymers (NiO4 -CCP NiN4 -CCP) with different motifs are investigated proof-of-concept study. The NiO4 exhibits yield rate as high 1.83 mmol h-1 mg-1 Faradaic efficiency 94.7% current density 125 mA cm-2 , outperforming catalyst. These experimental theoretical studies both suggest that can not only accelerate by adjusting adsorption energies intermediates on but also inhibit HER regulating migration contributions metal-hydrated cations adsorbed surface, thus achieving simultaneous enhancement activity.

Language: Английский

Citations

80
Metal–Organic Framework Supercapacitors: Challenges and Opportunities DOI Creative Commons
Seung‐Jae Shin, Jamie W. Gittins, Chloe J. Balhatchet

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(43)

Published: Sept. 17, 2023

Abstract Supercapacitors offer superior energy storage capabilities than traditional capacitors, making them useful for applications such as electric vehicles and rapid large‐scale storage. The performance of these devices relies on electrical double‐layer capacitance and/or pseudocapacitance from reversible redox reactions. Metal–organic frameworks (MOFs) have recently emerged a new class electrode materials with promising supercapacitor performances capacitances that exceed those materials. However, the comparison porous carbon state‐of‐the‐art MOF highlights number challenges supercapacitors, including low potential windows, limited cycle lifetimes, poor rate performances. It is proposed well‐defined tuneable chemical structures MOFs present avenues improving performance. Recent experimental theoretical work charging mechanisms in MOF‐based supercapacitors also discussed, it found there need more studies elucidate charge degradation mechanisms. Ultimately, deeper understanding will lead to design principles realizing improved devices.

Language: Английский

Citations

79
Bimetal‐Organic Framework Nanoboxes Enable Accelerated Redox Kinetics and Polysulfide Trapping for Lithium‐Sulfur Batteries DOI
Zhuo Zhu, Yinxiang Zeng, Zhihao Pei

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(31)

Published: June 7, 2023

Abstract Lithium‐sulfur (Li−S) batteries are considered as promising candidates for next‐generation energy storage systems in view of the high theoretical density and low cost sulfur resources. The suppression polysulfide diffusion promotion redox kinetics main challenges Li−S batteries. Herein, we design prepare a novel type ZnCo‐based bimetallic metal–organic framework nanoboxes (ZnCo‐MOF NBs) to serve functional host hollow architecture ZnCo‐MOF NBs can ensure fast charge transfer, improved utilization, effective confinement lithium polysulfides (LiPSs). atomically dispersed Co−O 4 sites firmly capture LiPSs electrocatalytically accelerate their conversion kinetics. Benefiting from multiple structural advantages, ZnCo‐MOF/S cathode shows reversible capacity, impressive rate capability, prolonged cycling performance 300 cycles.

Language: Английский

Citations

74