Regulating the Local Electronic Structure of Copper Single Atoms with Unsaturated B,O-Coordination for Selective ¹O₂ Generation

ACS Catalysis, Год журнала: 2023, Номер 13(18), С. 12414 - 12424

Опубликована: Сен. 7, 2023

Generating singlet oxygen (1O2) on single atom catalysts (SACs) in peroxymonosulfate (PMS)-based Fenton-like reactions exhibits great potential for selective degradation of contaminants complex wastewater. Clarifying the structure–activity relationship between electronic structure SACs and 1O2 generation selectivity is crucial precise design efficient catalysts, but it challenging. Herein, Cu with different structures (namely, Cu–O2X, where X = N, S, B, P, O) investigated by density functional theory calculations using adsorption terminal atoms PMS as an activity descriptor. Significantly, affected center which electron-depleted Cu-O2B site a higher atoms. Experimentally, moiety superior catalytic activation, showing nearly 100% ciprofloxacin rate 0.2250 min–1, outperforming those other counterparts. The high attributed to asymmetric accelerating faster electron transfer O–O bond stretching, lowering energy barrier key intermediates toward generation. This work provides broader perspective regulating sites at atomic level catalysts.

Язык: Английский

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Optimization strategies of high-entropy alloys for electrocatalytic applications

Chemical Science, Год журнала: 2023, Номер 14(45), С. 12850 - 12868

Опубликована: Янв. 1, 2023

This review summarizes the synthesis methods, characterization research progress and regulation strategies of HAEs in field electrocatalytic HER, HOR, OER, ORR, CO 2 RR, NRR AOR, providing deep understanding for future applications.

Язык: Английский

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Synthesis of MXene-based single-atom catalysts for energy conversion applications

Chemical Engineering Journal, Год журнала: 2023, Номер 474, С. 145700 - 145700

Опубликована: Сен. 1, 2023

Язык: Английский

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Atomic Distance Engineering in Metal Catalysts to Regulate Catalytic Performance

Advanced Materials, Год журнала: 2023, Номер 36(3)

Опубликована: Окт. 2, 2023

Abstract It is very important to understand the structure–performance relationship of metal catalysts by adjusting microstructure at atomic scale. The distance has an essential influence on composition environment active atom, which a key factor for design targeted with desired function. In this review, we discuss and summarize strategies changing from three aspects relate their effects reactivity catalysts. First, regulating bond length between coordination atom one single‐atom site catalytic performance are introduced. lengths affected strain effect support high‐shell doping can evolve during reaction. Next, sites discussed. Due space matching adsorption electron transport, be adjusted shortening distance. addition, arrangement spacing surface atoms nanocatalysts studied. Finally, comprehensive summary outlook given.

Язык: Английский

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Optimization Strategies of Covalent Organic Frameworks and Their Derivatives for Electrocatalytic Applications

Advanced Functional Materials, Год журнала: 2023, Номер 34(11)

Опубликована: Ноя. 27, 2023

Abstract Covalent organic frameworks (COFs) are crystalline porous polymers that can be precisely integrated by building blocks to achieve pre‐designed composition, components, and functions, making them a powerful platform for the development of molecular devices in field electrocatalysis. The precise control channel/dopant positions highly ordered network structures COFs provide an ideal material system applications advanced In this paper, topological structure design synthesis methods reviewed detail, their principles deeply analyzed. addition, derivatives electrocatalysis systematically summarized optimization strategies proposed. Finally, application prospects challenges may encountered future prospected, providing helpful guidance research.

Язык: Английский

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Dual-Atom Co/Ni Electrocatalyst Anchored at the Surface-Modified Ti₃C₂T_x MXene Enables Efficient Hydrogen and Oxygen Evolution Reactions

ACS Nano, Год журнала: 2024, Номер 18(5), С. 4256 - 4268

Опубликована: Янв. 24, 2024

Dual-atom catalytic sites on conductive substrates offer a promising opportunity for accelerating the kinetics of multistep hydrogen and oxygen evolution reactions (HER OER, respectively). Using MXenes as is strategy depositing those dual-atom electrocatalysts, if efficient surface anchoring ensuring metal-substrate interactions sufficient mass loading established. We introduce surface-modification MXene by preadsorbing L-tryptophan molecules, which enabled attachment Co/Ni electrocatalyst at Ti3C2Tx forming N–Co/Ni-O bonds, with reaching high 5.6 wt %. The electron delocalization resulting from terminated O atoms substrates, N in moieties, metal Co Ni provides an optimal adsorption strength intermediates boosts HER OER kinetics, thereby notably promoting intrinsic activity electrocatalyst. CoNi-Ti3C2Tx displayed overpotentials 31 241 mV 10 mA cm–2, respectively. Importantly, also exhibited operational stability both over 100 h industrially relevant current density 500 cm–2. Our study provided guidance constructing active to synergistically enhance electrochemical efficiency energy conversion storage systems.

Язык: Английский

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Self-supported transition metal chalcogenides for oxygen evolution

Nano Research, Год журнала: 2023, Номер 16(7), С. 8684 - 8711

Опубликована: Май 3, 2023

Язык: Английский

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Atomic Engineering of Single‐Atom Nanozymes for Biomedical Applications

Advanced Materials, Год журнала: 2024, Номер 36(21)

Опубликована: Фев. 7, 2024

Single-atom nanozymes (SAzymes) showcase not only uniformly dispersed active sites but also meticulously engineered coordination structures. These intricate architectures bestow upon them an exceptional catalytic prowess, thereby captivating numerous minds and heralding a new era of possibilities in the biomedical landscape. Tuning microstructure SAzymes on atomic scale is key factor designing targeted with desirable functions. This review first discusses summarizes three strategies for their impact reactivity biocatalysis. The effects choices carrier, different synthesis methods, modulation first/second shell, type number metal centers enzyme-like activity are unraveled. Next, attempt made to summarize biological applications tumor therapy, biosensing, antimicrobial, anti-inflammatory, other from mechanisms. Finally, how designed regulated further realization diverse reviewed prospected. It envisaged that comprehensive presented within this exegesis will furnish novel perspectives profound revelations regarding SAzymes.

Язык: Английский

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Exploring the potential Ru-based catalysts for commercial-scale polymer electrolyte membrane water electrolysis: A systematic review

Progress in Materials Science, Год журнала: 2024, Номер 145, С. 101294 - 101294

Опубликована: Апрель 5, 2024

Язык: Английский

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One-step growth of ultrathin CoSe2 nanobelts on N-doped MXene nanosheets for dendrite-inhibited and kinetic-accelerated lithium–sulfur chemistry

Science Bulletin, Год журнала: 2024, Номер 69(13), С. 2059 - 2070

Опубликована: Март 21, 2024

Язык: Английский

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