Multi‐Enzyme Mimetic MoCu Dual‐Atom Nanozyme Triggering Oxidative Stress Cascade Amplification for High‐Efficiency Synergistic Cancer Therapy DOI Open Access

Ziyao Li,

Binbin Ding, Jing Li

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 64(1)

Published: Aug. 22, 2024

Single-atom nanozymes (SAzymes) with ultrahigh atom utilization efficiency have been extensively applied in reactive oxygen species (ROS)-mediated cancer therapy. However, the high energy barriers of reaction intermediates on single-atom sites and overexpressed antioxidants tumor microenvironment restrict amplification oxidative stress, resulting unsatisfactory therapeutic efficacy. Herein, we report a multi-enzyme mimetic MoCu dual-atom nanozyme (MoCu DAzyme) various catalytic active sites, which exhibits peroxidase, oxidase, glutathione (GSH) nicotinamide adenine dinucleotide phosphate (NADPH) oxidase mimicking activities. Compared Mo SAzyme, introduction Cu atoms, formation synergetic effects among enhance substrate adsorption reduce barrier, thereby endowing DAzyme stronger Benefiting from above enzyme-like activities, can not only generate multiple ROS, but also deplete GSH block its regeneration to trigger cascade stress. Additionally, strong optical absorption near-infrared II bio-window endows remarkable photothermal conversion performance. Consequently, achieves high-efficiency synergistic treatment incorporating collaborative therapy This work will advance applications DAzymes provide valuable insights for nanocatalytic

Language: Английский

Recent advances of single-atom catalysts in CO2conversion DOI

Shunwu Wang,

Ligang Wang, Dingsheng Wang

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(7), P. 2759 - 2803

Published: Jan. 1, 2023

The catalytic transformation of CO 2 into valuable fuels/chemicals is a promising and economically profitable process because it offers an alternative toward fossil feedstocks the benefit transforming cycling on scale-up.

Language: Английский

Citations

144
Co-catalytic metal–support interactions in single-atom electrocatalysts DOI
Lucy Gloag, Samuel V. Somerville, J. Justin Gooding

et al.

Nature Reviews Materials, Journal Year: 2024, Volume and Issue: 9(3), P. 173 - 189

Published: Jan. 10, 2024

Language: Английский

Citations

123
Dinuclear metal synergistic catalysis for energy conversion DOI
Di‐Chang Zhong, Yun‐Nan Gong, Chao Zhang

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(9), P. 3170 - 3214

Published: Jan. 1, 2023

An exclusive review focusing on catalysts exhibiting the dinuclear metal synergistic catalysis (DMSC) effect for energy conversion reactions is presented.

Language: Английский

Citations

80
Single-atom Mo-tailored high-entropy-alloy ultrathin nanosheets with intrinsic tensile strain enhance electrocatalysis DOI Creative Commons
Lin He, Menggang Li,

Longyu Qiu

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: March 13, 2024

Abstract The precise structural integration of single-atom and high-entropy-alloy features for energy electrocatalysis is highly appealing conversion, yet remains a grand challenge. Herein, we report class Mo-tailored PdPtNiCuZn nanosheets with dilute Pt-Pt ensembles intrinsic tensile strain (Mo 1 -PdPtNiCuZn) as efficient electrocatalysts enhancing the methanol oxidation reaction catalysis. as-made Mo -PdPtNiCuZn delivers an extraordinary mass activity 24.55 A mg Pt −1 11.62 Pd+Pt , along impressive long-term durability. planted oxophilic single atoms promoters modify electronic structure isolated sites in host, suppressing formation CO adsorbates steering towards formate pathway. Meanwhile, synergistically optimize adsorption behaviour intermediates to achieve more energetically favourable pathway minimize barrier. This work advances design atomically catalytic by creating new paradigm atom-tailored high-entropy alloys, opening encouraging CO-tolerance electrocatalysts.

Language: Английский

Citations

79
Cobalt single atom anchored on N-doped carbon nanoboxes as typical single-atom catalysts (SACs) for boosting the overall water splitting DOI
Tong Li,

Siyuan Ren,

Cheng Zhang

et al.

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 458, P. 141435 - 141435

Published: Jan. 13, 2023

Language: Английский

Citations

72
Challenges and Perspectives of Single-Atom-Based Catalysts for Electrochemical Reactions DOI Creative Commons
Jiazhan Li, Chang Chen, Lekai Xu

et al.

JACS Au, Journal Year: 2023, Volume and Issue: 3(3), P. 736 - 755

Published: Feb. 16, 2023

Single-atom catalysts (SACs) are emerging as the most promising for various electrochemical reactions. The isolated dispersion of metal atoms enables high density active sites, and simplified structure makes them ideal model systems to study structure–performance relationships. However, activity SACs is still insufficient, stability usually inferior but has received little attention, hindering their practical applications in real devices. Moreover, catalytic mechanism on a single site unclear, leading development rely trial-and-error experiments. How can one break current bottleneck sites density? further increase activity/stability sites? In this Perspective, we discuss underlying reasons challenges identify precisely controlled synthesis involving designed precursors innovative heat-treatment techniques key high-performance SACs. addition, advanced operando characterizations theoretical simulations essential uncovering true electrocatalytic an site. Finally, future directions that may arise breakthroughs discussed.

Language: Английский

Citations

68
Oxygen Reduction Kinetics of Fe–N–C Single Atom Catalysts Boosted by Pyridinic N Vacancy for Temperature-Adaptive Zn–Air Batteries DOI
Lulu Lyu,

Hu Xu,

Suwon Lee

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(7), P. 4803 - 4813

Published: Feb. 9, 2024

The design of temperature-adaptive Zn–air batteries (ZABs) with long life spans and high energy efficiencies is challenging owing to sluggish oxygen reduction reaction (ORR) kinetics an unstable Zn/electrolyte interface. Herein, a quasi-solid-state ZAB designed by combining atomically dispersed Fe–N–C catalysts containing pyridinic N vacancies (FeNC-VN) polarized organo-hydrogel electrolyte. First-principles calculation predicts that adjacent VN sites effectively enhance the covalency Fe–Nx moieties moderately weaken *OH binding energies, significantly boosting ORR stability. In situ Raman spectra reveal dynamic evolution *O2– *OOH on FeNC-VN cathode in aqueous ZAB, proving 4e– associative mechanism dominant. Moreover, ethylene glycol-modulated electrolyte forms zincophilic protective layer Zn anode surface tailors [Zn(H2O)6]2+ solvation sheath, guiding epitaxial deposition Zn2+ (002) plane suppressing side reactions. assembled demonstrates span over 1076 h at 2 mA cm–2 −20 °C, outperforming most reported ZABs.

Language: Английский

Citations

66
Identification and Understanding of Active Sites of Non‐Noble Iron‐Nitrogen‐Carbon Catalysts for Oxygen Reduction Electrocatalysis DOI

Zhili Yang,

Yizhe Chen, Shiming Zhang

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(26)

Published: March 14, 2023

Non‐noble iron‐nitrogen‐carbon (Fe‐N‐C) catalysts have been explored as one type of the most promising alternatives precious platinum (Pt) in catalyzing oxygen reduction reaction (ORR). However, their catalytic ORR activity and stability still cannot meet requirement practical applications. Active sites such are key factors determining performance. This review gives a critical overview on identification understanding active sties non‐pyrolytic pyrolytic Fe‐N‐C terms design strategies, synthesis, characterization, functional mechanisms performance validation. The diversity complexity that greatly dominate progress include Fe‐containing (Fe‐based nanoparticles single‐atom Fe‐species) metal‐free (heteroatoms doping defects). Meanwhile, synergistic effects also discussed this with emphasis interaction among multiple sites. Although substantial endeavors devoted to develop efficient catalysts, some challenges remain. To facilitate further research toward applications, perspectives prospected aspects innovative synthesis methods, active‐sites modulation high‐resolution ex situ/in situ/operando characterization techniques, theoretical calculations, so on. may provide guideline for identifying developing high‐performance catalysts.

Language: Английский

Citations

55
Dual‐Atomic‐Site Catalysts for Molecular Oxygen Activation in Heterogeneous Thermo‐/Electro‐catalysis DOI

Zhongsen Wang,

Ming Cheng, Liu Yi

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(22)

Published: March 9, 2023

Efficient molecular oxygen activation (MOA) is the key to environmentally friendly catalytic oxidation reactions. In last decade, single-atomic-site catalysts (SASCs) with nearly 100 % atomic utilization and unique electronic structure have been widely investigated for MOA. However, single active site makes effect unsatisfactory difficult deal complex Recently, dual-atomic-site (DASCs) provided a new idea effective of (O2 ) due more diverse sites synergetic interactions among adjacent atoms. this review, we systematically summarized recent research progress DASCs MOA in heterogeneous thermo- electrocatalysis. Finally, look forward challenges application prospects construction

Language: Английский

Citations

54
Single-Atom-Based Oxygen Reduction Reaction Catalysts for Proton Exchange Membrane Fuel Cells: Progress and Perspective DOI
Jianmin Yu, Chenliang Su, Lu Shang

et al.

ACS Nano, Journal Year: 2023, Volume and Issue: 17(20), P. 19514 - 19525

Published: Oct. 9, 2023

Single-atom catalysts (SACs) are regarded as promising non-noble-metal alternatives for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells due to their high atom utilization efficiency and excellent catalytic properties. However, insufficient long-term stability issues of SACs under working conditions seriously hinder practical application. In this perspective, recent progress with optimized ORR activity is first reviewed. Then, possible degradation mechanisms process effective strategies improving durability summarized. Finally, some challenges opportunities proposed develop stable single-atom-based electrocatalysts future.

Language: Английский

Citations

51