Synergy of dual-atom catalysts deviated from the scaling relationship for oxygen evolution reaction DOI Creative Commons

Cong Fang,

Jian Zhou, Lili Zhang

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: July 24, 2023

Dual-atom catalysts, particularly those with heteronuclear active sites, have the potential to outperform well-established single-atom catalysts for oxygen evolution reaction, but underlying mechanistic understanding is still lacking. Herein, a large-scale density functional theory employed explore feasibility of *O-*O coupling mechanism, which can circumvent scaling relationship improving catalytic performance N-doped graphene supported Fe-, Co-, Ni-, and Cu-containing dual-atom namely, M'M@NC. Based on constructed activity maps, rationally designed descriptor be obtained predict homonuclear catalysts. Seven four possess high activities that minimum theoretical overpotential. The chemical structural origin in favor mechanism thus leading enhanced reaction been revealed. This work not only provides additional insights into fundamental mechanisms, also offers guideline accelerated discovery efficient

Language: Английский

Recent Progress on Two-Dimensional Materials DOI Open Access
Cheng Chang, Wei Chen, Ye Chen

et al.

Acta Physico-Chimica Sinica, Journal Year: 2021, Volume and Issue: 0(0), P. 2108017 - 0

Published: Jan. 1, 2021

Abstract: Research on two-dimensional (2D) materials has been explosively increasing in last seventeen years varying subjects including condensed matter physics, electronic engineering, science, and chemistry since the mechanical exfoliation of graphene 2004. Starting from graphene, 2D now have become a big family with numerous members diverse categories. The unique structural features physicochemical properties make them one class most appealing candidates for wide range potential applications. In particular, we seen some major breakthroughs made field five not only developing novel synthetic methods exploring new structures/properties but also identifying innovative applications pushing forward commercialisation. this review, provide critical summary recent progress particular focus years. After brief background introduction, first discuss materials, exfoliation, liquid vapor phase deposition, wet-chemical synthesis as well engineering belonging to nanomaterials (PEN). We then introduce superconducting/optical/magnetic chirality along newly emerging magic angle superlattices. Following that, promising electronics, optoelectronics, catalysis, energy storage, solar cells, biomedicine, sensors, environments, etc. are described sequentially. Thereafter, present theoretic calculations simulations materials. Finally, after concluding current progress, personal discussions existing challenges future outlooks rapidly field.

Language: Английский

Citations

379

Advances in the Development of Single‐Atom Catalysts for High‐Energy‐Density Lithium–Sulfur Batteries DOI
Ziwei Liang, Jiadong Shen, Xijun Xu

et al.

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(30)

Published: March 3, 2022

Abstract Although lithium–sulfur (Li–S) batteries are promising next‐generation energy‐storage systems, their practical applications limited by the growth of Li dendrites and lithium polysulfide shuttling. These problems can be mitigated through use single‐atom catalysts (SACs), which exhibit advantages maximal atom utilization efficiency (≈100%) unique catalytic properties, thus effectively enhancing performance electrode materials in devices. This review systematically summarizes recent progress SACs intended for Li‐metal anodes, S cathodes, separators, briefly introducing operating principles Li–S batteries, action mechanisms corresponding SACs, fundamentals activity, then comprehensively describes main strategies synthesis. Subsequently, operation reinforced as well other metal–S individually illustrated, major challenges usage future development directions presented.

Language: Английский

Citations

336

Atomically Dispersed Co2–N6 and Fe–N4 Costructures Boost Oxygen Reduction Reaction in Both Alkaline and Acidic Media DOI Creative Commons
Zhe Wang, Xiaoyan Jin, Chao Zhu

et al.

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(49)

Published: Oct. 8, 2021

Abstract Polynary transition‐metal atom catalysts are promising to supersede platinum (Pt)‐based for oxygen reduction reaction (ORR). Regulating the local configuration of atomic is key catalyst performance enhancement. Different from previously reported single‐atom or dual‐atom configurations, a new type ternary‐atom catalyst, which consists atomically dispersed, nitrogen‐coordinated Co–Co dimers, and Fe single sites (i.e., Co 2 –N 6 Fe–N 4 structures) that coanchored on highly graphitized carbon supports developed. This unique ORR outperforms with only in both alkaline acid conditions. Density functional theory calculations clearly unravels synergistic effect sites, can induce higher filling degree Fe–d orbitals favors binding capability *OH intermediates (the rate determining step). may be alternative Pt drive cathodic zinc–air batteries.

Language: Английский

Citations

314

A durable half-metallic diatomic catalyst for efficient oxygen reduction DOI
Hongguan Li,

Shuanlong Di,

Ping Niu

et al.

Energy & Environmental Science, Journal Year: 2022, Volume and Issue: 15(4), P. 1601 - 1610

Published: Jan. 1, 2022

By elaborately constructing a Fe–Zn based diatomic catalyst, the active center is changed from FeN 4– ZnN 4 to Zn–N 2 after protonation, leading well-maintained structure and thus high stability of ORR.

Language: Английский

Citations

220

Rational Design of Chemical Catalysis for Plastic Recycling DOI

Mingyu Chu,

Yu Liu,

Xiangxi Lou

et al.

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(8), P. 4659 - 4679

Published: April 5, 2022

Plastics are indispensable, but their pollution is triggering a global environmental crisis. Although many end-of-life catalytic options have involved converting plastics into valuable products, deep understanding of the relationship between polymer structure and recycling performance significant urgently needed. Here, we start with primer polymeric chain structures on chemical discuss structure–performance polymer, catalyst, reaction. Specifically, development challenges re/upcycling waste PET polyolefins discussed in-depth. In addition, also present some prospects for innovations in catalyst synthesis reaction engineering basis relationship. The discussion ends brief perspective future plastic re/upcycling. Overall, intelligent catalysis design necessary incentivizing relieving burden plastics.

Language: Английский

Citations

220

Understanding the Synergistic Effects of Cobalt Single Atoms and Small Nanoparticles: Enhancing Oxygen Reduction Reaction Catalytic Activity and Stability for Zinc‐Air Batteries DOI
Zhe Wang, Chao Zhu, Hua Tan

et al.

Advanced Functional Materials, Journal Year: 2021, Volume and Issue: 31(45)

Published: Aug. 8, 2021

Abstract The development of earth‐abundant oxygen reduction reaction (ORR) catalysts with high catalytic activity and good stability for practical metal‐air batteries remains an enormous challenge. Herein, a highly efficient durable ORR catalyst is reported, which consists atomically dispersed Co single atoms (Co‐SAs) in the form Co‐N4 moieties small nanoparticles (Co‐SNPs) co‐anchored on nitrogen‐doped porous carbon nanocage (Co‐SAs/SNPs@NC). Benefiting from synergistic effect Co‐SAs Co‐SNPs as well enhanced anticorrosion capability matrix brought by its improved graphitization degree, resultant Co‐SAs/SNPs@NC exhibits outstanding remarkable alkaline media, outperforming Co‐SAs‐based (Co‐SAs@NC), benchmark Pt/C catalyst. Density functional theory calculations reveal that strong interaction between sites can increase valence state active moderate adsorption free energy intermediates, thus facilitating O 2 . Moreover, zinc‐air battery assembled demonstrates maximum power density 223.5 mW cm –2 , specific capacity 742 W h kg –1 at 50 mA superior cycling stability.

Language: Английский

Citations

206

Recent advances in single atom catalysts for the electrochemical carbon dioxide reduction reaction DOI Creative Commons
Jincheng Zhang, Weizheng Cai,

Fang Hu

et al.

Chemical Science, Journal Year: 2021, Volume and Issue: 12(20), P. 6800 - 6819

Published: Jan. 1, 2021

The electrochemical carbon dioxide reduction reaction (CO2RR) offers a promising solution to mitigate emission and at the same time generate valuable carbonaceous chemicals/fuels. Single atom catalysts (SACs) are encouraging catalyze CO2RR due tunable electronic structure of central metal atoms, which can regulate adsorption energy reactants intermediates. Moreover, SACs form bridge between homogeneous heterogeneous catalysts, providing an ideal platform explore mechanism reactions. In this review, we first discuss strategies for promoting performance, including suppression hydrogen evolution (HER), generation C1 products formation C2+ products. Then, summarize recent developments in regulating toward based on above aspects. Finally, several issues regarding development raised possible solutions provided.

Language: Английский

Citations

192

Engineering 3d–2p–4f Gradient Orbital Coupling to Enhance Electrocatalytic Oxygen Reduction DOI

Xuan Wang,

Jingwen Wang, Pu Wang

et al.

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(42)

Published: Sept. 10, 2022

The development of highly efficient and economical materials for the oxygen reduction reaction (ORR) plays a key role in practical energy conversion technologies. However, intrinsic scaling relations exert thermodynamic inhibition on realizing active ORR electrocatalysts. Herein, novel feasible gradient orbital coupling strategy tuning performance through construction Co 3d-O 2p-Eu 4f unit sites Eu2 O3 -Co model is proposed. Through coupling, pristine ionic property between Eu O atoms assigned with increased covalency, which optimizes eg occupancy sites, weakens OO bond, thus ultimately breaking relation *OOH *OH at Co-O-Eu sites. optimized catalyst displays onset half-wave potential 1.007 0.887 V versus reversible hydrogen electrode, respectively, are higher than those commercial Pt/C most Co-based catalysts ever reported. In addition, found to possess superior selectivity durability. It also reveals better cell noble-metal Zn-air batteries terms high power/energy densities long cycle life. This study provides new perspective electronic modulation by 3d-2p-4f coupling.

Language: Английский

Citations

171

Graphene‐Supported Atomically Dispersed Metals as Bifunctional Catalysts for Next‐Generation Batteries Based on Conversion Reactions DOI
Biao Chen, Xiongwei Zhong, Guangmin Zhou

et al.

Advanced Materials, Journal Year: 2021, Volume and Issue: 34(5)

Published: Oct. 22, 2021

Next-generation batteries based on conversion reactions, including aqueous metal-air batteries, nonaqueous alkali metal-O2 and -CO2 metal-chalcogen metal-ion have attracted great interest. However, their use is restricted by inefficient reversible of active agents. Developing bifunctional catalysts to accelerate the reaction kinetics in both discharge charge processes urgently needed. Graphene-, or graphene-like carbon-supported atomically dispersed metal (G-ADMCs) been demonstrated show excellent activity various electrocatalytic making them promising candidates. Different from G-ADMCs for catalysis, which only require high one direction, rechargeable should provide discharging charging. This review provides guidance design fabrication next-generation reactions. The key challenges that prevent conversion, origin G-ADMCs, current principles highly analyzed highlighted each conversion-type battery. Finally, a summary outlook development G-ADMC materials with energy density efficiency are given.

Language: Английский

Citations

170

An efficient and durable trifunctional electrocatalyst for zinc–air batteries driven overall water splitting DOI
Natarajan Logeshwaran, S. Ramakrishnan, S. Selva Chandrasekaran

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2021, Volume and Issue: 297, P. 120405 - 120405

Published: June 1, 2021

Language: Английский

Citations

162