JOURNAL OF CATALYSIS
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2022
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IF 8.047
Xiaodong Zhang,Fukun Bi,Zhenyuan Zhao,Yang Yang,Yintao Li,Liang Song,Ning Liu,Jingcheng Xu,Lifeng Cui
Supported single-atoms and sub-nanometre clusters have exhibited superb catalytic performance toward many reactions. However, inactivation of single-atom or cluster catalysts in complex reactive conditions poses major challenge for their practical application. Herein, we demonstrate that the prepared Pd-UiO-66 with ultra-low Pd loading (0.05 wt%) contains three robust active Pd species, (isolated Pd atom (Pd 1 ), sub-nanometre Pd clusters (Pd c ) and Pd nanoparticles (Pd n )) and presents superb activity for toluene oxidation and water resistance (10.0 vol%). Experiments and theoretical calculations firstly confirm that consecutive H 2 -O 2 and reaction gas treatment (1000 ppm toluene in 20 vol.%O 2 /Ar) induce residual N species from solvent N, N-dimethylformamide to enter UiO-66 skeleton forming Pd 1 -N 1 structures. DFT calculations reveal that the synergistic effect of Pd species (namely, the enhanced activation of O 2 and H 2 O by Pd 1 and the improved adsorption of toluene by Pd c and Pd n ) is the main factor for the excellent activity of Pd-U-H-O-reused catalyst.
研究领域:
催化化学
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Zhijun Li,Honghong Li,Dundong Yuan,Leipeng Leng,Mingyang Zhang,Minghui Di,J. Hugh Horton,Jun Wang,Litao Sun,Weiwei Sun
Exploring the interaction between metal and support is of great importance in enhancing the catalytic performance and deepening the mechanistic understanding of single atom catalysis. Here we describe a photoinduction method to construct atomically dispersed palladium atoms supported over defect-containing boehmite (γ-AlOOH) nanoleaf with a palladium loading of 0.32 wt%. The existence of singly dispersed palladium atoms is confirmed by spherical aberration correction electron microscopy, extended X-ray absorption fine structure measurement, and CO-absorbed diffuse reflectance infrared Fourier transform spectroscopy. This catalyst shows excellent catalytic efficiency in trans -stilbene epoxidation to yield trans -stilbene oxide (TOF: 416 h −1 ; conversion: 84 %; selectivity: 99 %), along with excellent recyclability and scalability. In addition, various aromatic olefins were successfully transformed into the corresponding epoxides with high selectivity and excellent yield. DFT study further reveals that the high catalytic activity originates from under-coordinated single palladium atoms in the defect-containing γ-AlOOH in a unique coordination environment. This lays the foundation for the facile creation of single atom catalysts and sheds light on the possibility for scale-up production.
研究领域:
催化化学
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材料科学
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理论化学
✓ 已验证
产品关联
DOI
高影响因子
Science China-Materials
·
2023
·Vol. 66
·期 6
·2475-2482
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IF 8.1
Cai Chunqi,Chen Qingqing,Su Hongyan,Huang Pengcheng,Mao Junjie,Wu Fang-Ying
The detoxification of nerve agents, a class of extremely toxic chemical warfare agents, is urgently needed because they have remained a threat to humanity. To date, zirconium-based metal-organic frameworks (Zr-MOFs) are the most popular catalysts in this realm. However, it is still essential to develop new and efficient catalysts based on Zr-MOFs to achieve more rapid hydrolysis. Herein, we report that the single-atom catalyst (SAC) with Cu single atoms on a UiO-66-NH 2 support (Cu@UiO-66-NH 2 ) could significantly boost the degradation of the nerve agent simulant. Compared with the pristine UiO-66-NH 2 , this SAC exhibited remarkable catalytic activity with a half-life for hydrolysis of ∼2 min and better reusability in cyclic experiments. Both experimental and theoretical studies suggest that the atomically dispersed Cu species anchored to the amino groups rather than to the Zr 6 node of UiO-66-NH 2 acted as the catalytic active sites, leading to favorable binding geometries with the substrate and the product. A catalytic mechanism on the SAC different from that generally considered on the pristine Zr-MOFs was thus presented to elucidate the enhanced catalytic efficiency.
研究领域:
化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Pharmaceutics
·
2023
·Vol. 15
·期 4
·1217
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IF 5.4
Tushuai Li,Yue Gu,Lisha Yu,Shenglong Zhu,Jie Zhang,Yongquan Chen
Tumor microenvironment (TME)-induced nanocatalytic therapy is a trending strategy for tumor-targeting therapy, but the low catalytic efficiency remains to limit its therapeutic effect. The single-atom catalysts (SACs) appear as a novel type of nanozymes that possesses incredible catalytic activity. Here, we developed PEGylated manganese/iron-based SACs (Mn/Fe PSACs) by coordinating single-atom Mn/Fe to nitrogen atoms in hollow zeolitic imidazolate frameworks (ZIFs). Mn/Fe PSACs catalyze cellular hydrogen peroxide (H2O2) converting to hydroxyl radical (•OH) through a Fenton-like reaction; it also enhances the decomposition of H2O2to O2that continuously converts to cytotoxic superoxide ion (•O2−) via oxidase-like activity. Mn/Fe PSACs can reduce the depletion of reactive oxygen species (ROS) by consuming glutathione (GSH). Here, we demonstrated the Mn/Fe PSACs-mediated synergistic antitumor efficacy among in vitro and in vivo experiments. This study proposes new promising single-atom nanozymes with highly efficient biocatalytic sites and synergistic therapeutic effects, which will give birth to abundant inspirations in ROS-related biological applications in broad biomedical fields.Keywords:tumor microenvironment;single-atom catalysts;reactive oxygen species;synergistic antitumor
研究领域:
纳米技术
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癌症生物学
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生物医学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Kaiyang Xu,Yu Chen,Hua Yang,Yuyan Gan,Lizhi Wu,Li Tan,Yihu Dai,Yu Tang
Cyclohexanone is an important raw material for manufacturing nylon and other chemicals. The sustainable conversion of biomass derived molecules to cyclohexanone is desired but still challenging. Herein, a palladium single atom catalyst anchored in the micropores of zeolite (namely Pd 1 /ZSM-5) is designed and exhibits remarkable catalytic activity in transforming anisole to cyclohexanone in water medium (H 2 O), without using of organic solvent or halogen promoter. The selectivity to cyclohexanone is 91.2% and the turnover rate (TOR) is 400.8 h −1 at 453 K. The Pd sites, acid sites, and microporous confinement environment of zeolite cooperate to promote the partial hydrogenation to cyclohexanone, and inhibit further hydrogenation as the side reaction. H 2 O not only acts as the solvent, but also participates significantly in the partial hydrogenation. Moreover, as revealed by isotope labelled experiments (D 2 O and H 2 18 O), the water participated hydrogenolysis and the consequent partial hydrogenation mechanism is proposed.
研究领域:
催化化学
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绿色化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Quan Quan,Zhang Yuxuan,Li Haifan,Wang Wei,Xie Pengshan,Chen Dong,Wang Weijun,Meng You,Yin Di,Li Yezhan,Song Dongyuan,Chen Lijie,Li Shaohai,Yang Cheng,Yanagida Takeshi,Wong Chun-Yuen,Yip SenPo,Ho Johnny C.
Maximizing metal-substrate interactions by self-reconstruction of coadjutant metastable phases can be a delicate strategy to obtain robust and efficient high-density single-atom catalysts. Here, we prepare high-density iridium atoms embedded ultrathin CoCeOOH nanosheets (CoCe-O-Ir SA ) by the electrochemistry-initiated synchronous evolution between metastable iridium intermediates and symmetry-breaking CoCe(OH) 2 substrates. The CoCe-O-Ir SA delivers an overpotential of 187 mV at 100 mA cm −2 and a steady lifespan of 1000 h at 500 mA cm −2 for oxygen evolution reaction. Furthermore, the CoCe-O-Ir SA is applied as a robust anode in an anion-exchange-membrane water electrolysis cell for seawater splitting at 500 mA cm −2 for 150 h. Operando experimental and theoretical calculation results demonstrate that the reconstructed thermodynamically stable iridium single atoms act as highly active sites by regulating charge redistribution with strongly p - d - f orbital couplings, enabling electron transfer facilitated, the adsorption energies of intermediates optimized, and the surface reactivity of Co/Ce sites activated, leading to high oxygen evolution performance. These results open up an approach for engineering metastable phases to realize stable single-atom systems under ambient conditions toward efficient energy-conversion applications.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
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2025
·Vol. 16
·期 1
·1-13
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IF 15.7
Guo Wei,Pan Meiling,Xie Qianjie,Fan Hua,Luo Laihao,Jing Qun,Shen Yehua,Yan Yan,Liu Mingkai,Wang Zheng
Renewable biomass serves as a cost-effective source of carbon matrix to carry single-atom catalysts (SACs). However, the natural abundant oxygen in these materials hinders the sufficient dispersion of element with high oxygen affinity such iron (Fe). The lowered-density and oxidized SACs greatly limits their catalytic applications. Here we develop a facile continuous activation (CA) approach for synthesizing robust biomass-derived Fe-SACs. Comparing to the traditional pyrolysis method, the CA approach significantly increases the Fe loading density from 1.13 atoms nm −2 to 4.70 atoms nm −2 . Simultaneously, the CA approach induces a distinct coordination tuning from dominated Fe-O to Fe-N moieties. We observe a pH-universal oxygen reduction reaction (ORR) performance over the CA-derived Fe-SACs with a half-wave potential of 0.93 V and 0.78 V vs. RHE in alkaline and acidic electrolyte, respectively. Density functional theory calculations further reveal that the increased Fe-N coordination effectively reduces the energy barriers for the ORR, thus enhancing the catalytic activity. The Fe-SACs-based zinc-air batteries show a specific capacity of 792 mA·h·g Zn −1 and ultra-long life span of over 650 h at 5 mA cm −2 .
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Wang Zhigui,Lu Guolong,Wei Tianran,Meng Ge,Cai Haoxiang,Feng Yanhong,Chu Ke,Luo Jun,Hu Guangzhi,Wang Dingsheng,Liu Xijun
Aqueous redox flow batteries (RFBs) incorporating polysulfide/iodide chemistries have received considerable attention due to their safety, high scalability, and cost-effectiveness. However, the sluggish redox kinetics restricted their output energy efficiency and power density. Here we designed a defective MoS 2 nanosheets supported Co single-atom catalyst that accelerated the transformation of S 2− /S x 2− and I − /I 3 − redox couples, hence endow the derived polysulfide–iodide RFB with an initial energy efficiency (EE) of 87.9% and an overpotential of 113 mV with an average EE 80.4% at 20 mA cm −2 and 50% state-of-charge for 50 cycles, and a maximal power density of 95.7 mW cm −2 for an extended cycling life exceeding 850 cycles at 10 mA cm −2 and 10% state-of-charge. In situ experimental and theoretical analyses elucidate that Co single atoms induce the generation of abundant sulfur vacancies in MoS 2 via a phase transition process, which synergistically contributed to the enhanced adsorption of reactants and key reaction intermediates and improved charge transfer, resulting in the enhanced RFB performance.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Chem Catalysis
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2024
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IF 11.5
Fei-Yang Yu,Hao Sun,Hua-Qiao Tan,Yang-Guang Li,Shuit-Tong Lee,Zhen-Hui Kang
The dynamic evolution and structure-performance relationships of single-atom catalysts (SACs) under operating conditions are one of the most concerned hotspots at present. Here, we employed Anderson-type polyoxometalates as a precursor to prepare the SAC Rh-MoS 2 , which shows excellent hydrogen evolution reaction (HER) performance with a mass activity of 4.26 A mg −1 at 100 mV. Such a result is much better than that of 20% Pt/C. Extensive experimental characterization combined with density functional theory (DFT) calculations suggest that the active site undergoes a dynamic evolution from Rh-S to Rh-S/O, while at the same time, the support is transformed from 1T MoS 2 to 1T-2H MoS 2 . It is this dynamic evolution of the catalyst structure that causes a series of changes in the activity, and eventually, a balance between catalytic activity and stability is achieved. This work offers a good research demonstration of the dynamic evolution of SACs under operating conditions and provides a new perspective on the design of SACs.
研究领域:
材料科学
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理论化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Longjian Li,Junhui Wang,Qinhua Zhang,Shuai Wang,Hangkai Zhang,Tao Xing,Mingqing Wang,Mingbo Wu,Zhenxing Wang,Wenting Wu
Near-infrared light occupies 54.3% of the solar spectrum and has greater penetration depth, and its effective utilization is of great significance in the practical application of photocatalysis on a larger scale. However, the development of catalysts that can directly utilize near-infrared light is still a huge challenge. This paper proposes a strategy to directly utilize near-infrared light (excitation wavelength extending to 850 nm) by creating carbon material doped with a high-spin-state Co(II)-Nx single-atom site. In the near-infrared-light-irradiated photooxidation of 1,5-dihydroxynaphthalene, the yield of juglone can reach 45% without a significant decrease, even when the catalytic volume is increased by 20 times, which was much higher than that irradiated by 460 nm wavelength (reduced by about 23%). Our study sets the stage for fabricating stable NIR photocatalysts and provides a solution to directly enhance NIR photooxidation in a large-scale manner.
研究领域:
材料科学
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光化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2024
·
IF 5.8
Fenghui Li,Xuhui Li,Yawei Jiang,Yingjie Cao,Wenjian Fang,Tao Zhou,Jiang Wu,Yongsheng Liu
Photocatalysis has gained significant attention in recent years for water splitting, with graphitic carbon nitride (g-C 3 N 4 ) emerging as a promising candidate. However, the low carrier mobility and the lack of active sites for hydrogen evolution limit photocatalytic hydrogen evolution performance. Herein, this work presents a facile approach to achieve single Mo sites with a unique local coordination structure featuring one Mo atom coordinated with two nitrogen atoms and one sulfur atom . Among the prepared photocatalysts , 6 wt % Mo/SCN exhibits the highest photocatalytic hydrogen evolution activity with a yield rate of 4.05 mmol g -1 h -1 , which is 13 times higher than that of pure g-C 3 N 4 and superior to most of the g-C 3 N 4 series photocatalysts. Experimental results and density functional theory calculations confirm that the Mo single-atom and S atom have synergistic catalysis under the co-modification, and the formed Mo-S bonds will enhance the ability of the substrate to anchor the Mo single-atom to enhance the stability of the photocatalyst. This work offers insights into transition metal single-atom and synergistic catalysis design for photocatalytic hydrogen evolution.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
CRYSTENGCOMM
·
2024
·
IF 2.6
Zikun Yang,Jingxuan Zheng,shi mengge,Zhao Wang
Single-atom catalysts (SACs) have attracted significant attention due to their unique electronic structure and extraordinary catalytic reaction activity. In this work, the single-atom catalysts Au1/TiO2 were successfully prepared using cold plasma. Notably, plasma-treated TiO2 introduces a substantial number of oxygen vacancies, which played a confinement effect on gold atoms. Au1/TiO2 achieved a remarkable 67% degradation of RhB in just 120 minutes, surpassing the performance of AuNPs/TiO2 by 2.8 times. The high catalytic activity can be attributed to several factors. Firstly, plasma-treated TiO2 contained a higher density of oxygen vacancies and exhibited a narrower band gap, which improved light absorption and facilitated the anchoring of monoatomic Au on the catalyst surface. Additionally, the single-atom Au species exhibited stronger interactions with TiO2, enhancing light absorption and charge transfer capability. Simultaneously, the presence of SACs on the catalyst surface increased the number of active sites, promoting efficient separation of electron-hole pairs and consequently enhancing the photocatalytic degradation activity. Cold plasma technology offers a simple and environmentally friendly platform for the fabrication of SACs, opening up exciting possibilities for catalytic applications.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）