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
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产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
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
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产品关联
DOI
PubMed
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
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产品关联
DOI
PubMed
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
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
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产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Zhounan Yu,Leilei Zhang,Yuanlong Tan,Rizheng Jing,Hongchen Cao,Caiyi Lou,Rile Ge,Junhu Wang,Aiqin Wang,Tao Zhang
Rh-P complexes have been widely used as catalysts for hydroformylation reactions. The extremely high price of Rh and its scarce reserves have prompted the exploration of the alternatives. In this study, we reported that Pt/PS-PPh 2 single-atom catalysts promoted by SnCl 2 were highly efficient and selective for the hydroformylation of higher α-alkenes. A broad scope of substrates (i.e., C 6 –C 12 ) were smoothly converted to the corresponding linear aldehydes with high yields under reaction conditions of 90–120 °C and 4–6 MPa syngas . The turnover frequency (TOF) was comparable to homogeneous Pt-Sn catalysts, and the linear/branched ratio reached as high as > 20. In addition, the catalyst could be reused with the extra addition of SnCl 2 . The promotional role of SnCl 2 was elucidated by quasi- in situ X-ray adsorption fine structure, Fourier transform infrared, and Mössbauer spectroscopy . It was discovered that SnCl 2 was transformed into Sn(dioxane)Cl 3 − species coordinated to Pt as a moderately electron-donating ligand, which, together with the phosphine group, stabilized mononuclear Pt (I) species against reduction and aggregation.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Haoquan Guo,Jiwu Zhao,Yu Chen,Xinyu Lu,Yue Yang,Chenrong Ding,Lizhi Wu,Li Tan,Jinlin Long,Guohui Yang,Yu Tang,Noritatsu Tsubaki,Xiaoli Gu
Lignin derivatives are one class of attractive alternative feedstocks for the production of renewable biofuels. Herein, hydrodeoxygenation (HDO) of lignin derivatives was carried out using a single-atom catalyst (SAC) comprised of Ni1 SAC on β-Mo2C. A number of lignin-derived compounds have been investigated, and nearly 100% yield of biofuel molecules was converted from various lignin derivatives through the HDO reaction, demonstrating that Ni1/β-Mo2C has remarkable potential for the production biofuels through catalytic hydrodeoxygenation of lignin derivatives. The reaction mechanism of DHE over single-atom catalyst Ni1/β-Mo2C was confirmed based on comprehensive characterizations of catalysts and DFT calculations. Interestingly, the Ni single-atom active sites alter the reaction pathway by shifting the geometry of the adsorbed intermediate from a vertical to horizontal conformation, which lowered the reaction energy barrier and improved the selectivity to biofuel molecules, resulting in extraordinary catalytic activity. This study suggests an avenue for single-atom catalysis in chemical transformations of lignin derivatives into biofuels.
研究领域:
化学工程
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催化科学
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可再生能源
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产品关联
DOI
高影响因子
Nano-Micro Letters
·
2024
·Vol. 17
·期 1
·1-17
·
IF 31.6
Chen Si,Huang Fang,Mao Lijie,Zhang Zhimin,Lin Han,Yan Qixin,Lu Xiangyu,Shi Jianlin
Fe single-atom catalysts (h 3 -FNCs) with high loading, high catalytic activity and high stability were synthesized via a method capable of increasing both the metal loading and mass-specific activity by exchanging zinc with iron.
The “density effect,” derived from the sufficiently high density of active sites, has been discovered for the first time, leading to a significant alteration in the intrinsic activity of single-atom metal sites.
The superior oxidase-like catalytic performance of h 3 -FNCs ensures highly effective bacterial eradication.
研究领域:
生物医学工程
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材料科学
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产品关联
DOI
PubMed
高影响因子
FUEL
·
2022
·
IF 8.035
Zezhong Cao,Panpan Su,Xinyao Wang,Xiaoyan Liu,Yanfu Ma,Congming Li,San Ping Jiang,Jian Liu
Single-site metal catalysts (SSMCs) with high activity and stability have been widely applied as electrocatalysts for electrochemical CO 2 reduction reaction (CO 2 RR) process. However, it remains challenging for precise controlling the nanoarchitectures and atomic metal sites of SSMCs to investigate their corresponding structural and related catalytic properties toward CO 2 RR. In this work, four categories of Ni based SSMCs with different nanoarchitectures were successfully synthesized, including Ni-N doped solid carbon spheres with micropore (Ni-N/C-S-Micro), Ni-N doped hollow carbon spheres with micropore (Ni-N/C–H-Micro), Ni-N doped hollow carbon spheres with mesopore (Ni-N/C–H-Meso), and Ni-N doped hollow carbon spheres with micropore and mesopore (Ni-N/C–H-Micro/Meso). Ni-N/C-S-Micro and Ni-N/C–H-Micro were favorable for the generation of atomic Ni sites in SSMCs, resulting in higher loading amount of Ni, while Ni-N/C–H-Meso with open structure leads to the aggregation of Ni species during pyrolysis. In comparison with Ni-N/C-S-Micro, carbon spheres with hollow and mesoporous structures can enhance the diffusion of CO 2 and improve the catalytic activity of per Ni site toward CO 2 RR process. Thus, Ni-N/C–H-Meso shows the highest turnover frequencies (TOF) value for CO 2 RR to CO. This study provides a SSMCs design protocol for investigation the SSMCs correlation of structure and properties toward electrochemical conversions.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Huiyuan Cheng,Xuemei Wu,Xiangcun Li,Xiaowa Nie,Shuai Fan,Manman Feng,Zihao Fan,Mingqian Tan,Yonggang Chen,Gaohong He
Although considerable progress has been achieved by Cu nanoparticles for catalyzing CO 2 reduction reaction (CO2RR), Cu single atom catalysts (Cu SACs) are generally suffered from inferior performance to that of widely investigated Fe, Co, Ni SACs. This phenomenon mainly ascribes to the lack of effective geometry and electronic engineering of copper active center from an atomic level. Herein, highly exposed atomically dispersed Cu-N x ( x denotes Cu–N coordination number) sites anchored on 3D porous carbon matrix are successfully synthesized through facile one step thermal activation, and Cu-N 4 sites exhibit boosted activity and selectivity compared to its nearly inert Cu-N 3 counterparts. Aided by density functional theory (DFT) calculations, the edge-hosted Cu-N 4 moieties are revealed as key active sites for efficient CO generation via optimized local coordination environment and electronic properties, which strongly interact with *COOH intermediate and facilitate the desorption of *CO. As a result, Cu-N 4 catalyst achieves high CO Faradaic efficiency (FE CO ) of over 90% from −0.6 to −1.1 V vs . RHE with a maximum value of 98%, surpassing the previously reported Cu SACs for CO 2 -to-CO conversion. This work provides new insight into proper Cu SACs design and fundamental mechanism understanding to boost CO2RR.
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
高影响因子
CHEMPHYSCHEM
·
2022
·Vol. 24
·期 7
·e202200505
·
IF 3.52
Xujun Ma,Donghui Wang,Jianan Wu,Bin Zhao,Feng Chen
Graphical Fe 3+ doping was utilized to promote the formation of oxygen vacancies and improve the interaction between TiO 2 and atomic Pt. Single Pt atoms anchored on the oxygen vacancy sites of Fe−TiO 2 effectively modify the local energy band structure of TiO 2 , and thus significantly boost the catalytic performance of either the intrinsic or the sensitized photocatalytic process for Pt/Fe−TiO 2 . Single atomic site catalysts display the maximal atom-utilization efficiency, unique structural properties, and remarkable enhancements on catalytic activity. Herein, single Pt atoms loaded Fe−TiO 2 catalysts were prepared. Fe 3+ doping leads to the formation of oxygen vacancies and improve the interaction between TiO 2 and Pt. Single Pt atoms are thus anchored and effectively modify the local energy band structure of TiO 2 . The optimized local band structures improve the intrinsic photoexcitation of Pt/Fe−TiO 2 , promote the separation of photogenerated carriers, and extend the lifetime of photogenerated carriers. Meanwhile, the electrons transfer from the excited dyes to the conduction band edge of Pt/Fe−TiO 2 is also facilitated due to the shift-down of the conduction band edge. Therefore, with the increase of the Pt content (till up to 0.6 wt%), the photocatalytic performance of Pt/ Fe−TiO 2 with the confined single Pt atoms is significantly boosted in either the intrinsic or the sensitized photocatalytic process.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yi Yu,Yu Cheng,Lei Tan,Xiangmei Liu,Zhaoyang Li,Yufeng Zheng,Tao Wu,Yanqin Liang,Zhenduo Cui,Shengli Zhu,Shuilin Wu
Periodontitis is a chronic inflammatory disease caused by the bacteria infection in dental plaque, which can lead to gingival recession and tooth loss, seriously endangering human oral health. Current treatments through the combination of mechanical debridement and antibiotics therapy still have the problems of gingival trauma, low treatment efficiency, long treatment cycle and bacterial resistance. Herein, we prepare an injectable ointment based on MOF-based single-atom catalysis systems with good biocompatibility and high anti-biofilm activity, which consists of PEG-400/PEG-4000 and Pt single-atom doped porphyrin metal−organic framework (PCN-222-Pt). Through theoretical screening, we find that all the metal single atoms (Pt, Au, Cu, Ru) can improve the oxidase-like activity of PCN-222, which reduce the adsorption and activation energy of O 2 . Among them, PCN-222-Pt shows strong oxidase-like and peroxidase-like activities and can produce reactive oxygen species spontaneously, which shows an excellent anti-biofilm performance (98.69% against S. aureus biofilm, 99.91% against E. coli biofilm) in vitro within 1 h. In the treatment of biofilm-induced periodontitis, the injectable PCN-222-Pt ointment showed alleviative inflammation response, reduced bone destruction and healthier gum tissue, which is superior to the clinical used Periocline. This work provides a rapid, effective, non-invasive and convenient strategy for the treatment of periodontitis without antibiotics.
研究领域:
口腔医学
·
材料科学
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微生物学
✓ 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）