High‐Throughput Screening and General Synthesis Strategy of Single‐Atom Nanozymes for Oral Squamous Cell Carcinoma Therapy DOI Open Access

Ji Shen,

Guan-Meng Zhang,

Zedong Zhang

et al.

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 5, 2025

Abstract Single‐atom nanozymes (SAzymes), with their superior enzyme‐like catalytic activity, have emerged as promising candidates for oncology therapeutics. The well‐defined structures of SAzymes make them well predictable by experiences and theoretical calculation. However, the effects metal center species coordination environments on activity are variable, screening artificial experiments is challenging. High‐throughput can rapidly select optimal thus better application in tumor therapy highly desirable. Herein, a “high‐throughput screening‐SAzymes structures” system established efficient drug preparation density functional theory oxidase‐like processes screened differences brought about different metals environments. Through this process, transition (Mn, Fe, Co, Ni) active centers synthesized then tested multi‐enzyme activities. It found that SAzyme Co exhibited best further showed good anti‐oral squamous cell carcinoma properties both vitro vivo. This study opens up new avenue rational design oral cancer combining computational experimental validation.

Language: Английский

Self-carbon-thermal-reduction strategy for boosting the Fenton-like activity of single Fe-N4 sites by carbon-defect engineering DOI Creative Commons
Shengjie Wei,

Yibing Sun,

Yun-Ze Qiu

et al.

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

Published: Nov. 20, 2023

Carbon-defect engineering in metal single-atom catalysts by simple and robust strategy, boosting their catalytic activity, revealing the carbon defect-catalytic activity relationship are meaningful but challenging. Herein, we report a facile self-carbon-thermal-reduction strategy for carbon-defect of single Fe-N4 sites ZnO-Carbon nano-reactor, as efficient catalyst Fenton-like reaction degradation phenol. The vacancies easily constructed adjacent to during synthesis, facilitating formation C-O bonding lowering energy barrier rate-determining-step Consequently, Fe-NCv-900 with exhibits much improved than Fe-NC-900 without abundant vacancies, 13.5 times improvement first-order rate constant phenol degradation. shows high (97% removal ratio only 5 min), good recyclability wide-ranging pH universality (pH range 3-9). This work not provides rational improving catalysts, also deepens fundamental understanding on how periphery environment affects property performance metal-N4 sites.

Language: Английский

Citations

70
Sabatier Phenomenon in Hydrogenation Reactions Induced by Single-Atom Density DOI
Hongqiang Jin,

Runqing Zhao,

Peixin Cui

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(22), P. 12023 - 12032

Published: May 26, 2023

The Sabatier principle is a fundamental concept in heterogeneous catalysis that provides guidance for designing optimal catalysts with the highest activities. For first time, we here report new phenomenon hydrogenation reactions induced by single-atom density at atomic scale. We produce series of Ir (SACs) predominantly Ir1-P4 coordination structure densities ranging from 0.1 to 1.7 atoms/nm2 through P-coordination strategy. When used as hydrogenation, volcano-type relationship between and activity emerges, summit moderate 0.7 atoms/nm2. Mechanistic studies show balance adsorption desorption strength activated H* on single atoms found be key factor phenomenon. transferred Bader charge these SACs proposed descriptor interpret structure-activity relationship. In addition, maximum selectivity can simultaneously achieved chemoselective optimized catalyst due uniform geometric electronic structures sites SACs. present study reveals an insightful rational design more efficient practicable reactions.

Language: Английский

Citations

66
Metal and Metal Oxide Supported on Ordered Mesoporous Carbon as Heterogeneous Catalysts DOI

Meiqi Gao,

Lili Wang,

Yang Yang

et al.

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(7), P. 4060 - 4090

Published: March 9, 2023

The evolution of model catalyst systems has experienced single-crystal surfaces different transition metals and crystal faces, two-dimensional with nanoparticles (NPs) deposited on a flat support surface, three-dimensional NPs loaded into the high-surface-area supports such as ordered mesoporous materials. latter two mimic nanoparticle properties in industrial catalysts. Ordered carbon (OMC) materials play unparalleled roles catalysis, energy storage, adsorption, chromatographic separation, etc. because their distinctive structure which allows Knudsen diffusion inside mesopores, dispersion oxides, embedment pore walls. In this review, synthesis routes OMC-supported metal or oxide catalysts, including hard-templating soft-templating methods, are briefly introduced. Mass transfer reactant chemisorption metals, discrimination active species, catalytic reaction mechanism catalysts systemically summarized, highlight advantages catalysis occurring mesopores. Understanding these molecular-dominated factors provides insight controlling highly selective reactions and, therefore, design long life.

Language: Английский

Citations

63
State-of-the-art single-atom catalysts in electrocatalysis: From fundamentals to applications DOI
Muhammad Humayun, Muhammad Israr, Abbas Khan

et al.

Nano Energy, Journal Year: 2023, Volume and Issue: 113, P. 108570 - 108570

Published: May 29, 2023

Language: Английский

Citations

59
High‐Throughput Screening of Electrocatalysts for Nitrogen Reduction Reactions Accelerated by Interpretable Intrinsic Descriptor DOI
Xiaoyun Lin, Yongtao Wang, Xin Chang

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(19)

Published: March 9, 2023

Developing easily accessible descriptors is crucial but challenging to rationally design single-atom catalysts (SACs). This paper describes a simple and interpretable activity descriptor, which obtained from the atomic databases. The defined descriptor proves accelerate high-throughput screening of more than 700 graphene-based SACs without computations, universal for 3-5d transition metals C/N/P/B/O-based coordination environments. Meanwhile, analytical formula this reveals structure-activity relationship at molecular orbital level. Using electrochemical nitrogen reduction as an example, descriptor's guidance role has been experimentally validated by 13 previous reports well our synthesized 4 SACs. Orderly combining machine learning with physical insights, work provides new generalized strategy low-cost while comprehensive understanding structure-mechanism-activity relationship.

Language: Английский

Citations

52
Tailoring the Electronic Structure of Single Ag Atoms in Ag/WO3 for Efficient NO Reduction by CO in the Presence of O2 DOI
Yongjun Ji, Xiaoli Chen, Shaomian Liu

et al.

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(2), P. 1230 - 1239

Published: Jan. 5, 2023

Developing efficient catalysts for the selective catalytic reduction of NOx by CO (CO-SCR) is key challenge commercializing this technology. Ag-based with relatively low costs are promising but widely believed to be not enough reaction. Here, we demonstrate that atomically dispersed Ag supported on ordered mesoporous WO3 (m-WO3) can serve as a highly active catalyst CO-SCR under O2-containing conditions. By altering amount precursor, local environment atom coordinated O tailored. Furthermore, at 250 °C and an O2/CO ratio 2.5:1, 0.3Ag/m-WO3 (0.3 wt % Ag) six-coordinated Ag–O exhibited much better performance than 5 Ag/m-WO3 (5 two-coordinated (e.g., 0.43 vs 0.02 molNO gAg–1 h–1 in reaction rate) previously reported literature. The theoretical calculations confirm atoms possess more positive oxidation state higher d-band center 5Ag/m-WO3, promoting its bonding strength co-adsorption critical intermediates N2O* CO*. This work provides feasible route regulating single atomic enhance property CO-SCR.

Language: Английский

Citations

45
Surface Engineered Single‐atom Systems for Energy Conversion DOI

Yutang Yu,

Zijian Zhu, Hongwei Huang

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(16)

Published: Jan. 10, 2024

Abstract Single‐atom catalysts (SACs) are demonstrated to show exceptional reactivity and selectivity in catalytic reactions by effectively utilizing metal species, making them a favorable choice among the different active materials for energy conversion. However, SACs still early stages of conversion, problems like agglomeration low conversion efficiency hampering their practical applications. Substantial research focus on support modifications, which vital SAC stability due intimate relationship between atoms support. In this review, category supports variety surface engineering strategies employed SA systems summarized, including site (heteroatom doping, vacancy introducing, groups grafting, coordination tunning) structure (size/morphology control, cocatalyst deposition, facet engineering, crystallinity control). Also, merits single‐atom systematically introduced. Highlights comprehensive summary discussions utilization surface‐engineered diversified applications photocatalysis, electrocatalysis, thermocatalysis, devices. At end potential obstacles using field discussed. This review aims guide rational design manipulation target‐specific capitalizing characteristic benefits engineering.

Language: Английский

Citations

29
Hierarchically stabilized Pt single-atom catalysts induced by an atomic substitution strategy for an efficient hydrogen evolution reaction DOI

Changle Yue,

Chao Feng,

Guangxun Sun

et al.

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(14), P. 5227 - 5240

Published: Jan. 1, 2024

Tuning and stabilizing the chemical microenvironment of Pt-based single-atom catalysts is a major challenge in promoting an electrocatalytic hydrogen evolution reaction (HER).

Language: Английский

Citations

27
Tuning the local coordination environment of single-atom catalysts for enhanced electrocatalytic activity DOI

Wenhao Feng,

Chunli Liu, Guangxun Zhang

et al.

EnergyChem, Journal Year: 2024, Volume and Issue: 6(2), P. 100119 - 100119

Published: Feb. 17, 2024

Language: Английский

Citations

26
Precisely manipulating the local coordination of cobalt single-atom catalyst boosts selective hydrogenation of nitroarenes DOI
Fengliang Cao,

Wanxin Ni,

Qingshan Zhao

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 346, P. 123762 - 123762

Published: Jan. 20, 2024

Language: Английский

Citations

24