ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Yunjia Wei,Qi Hao,Xingce Fan,Mingze Li,Lei Yao,Guoqun Li,Xing Zhao,Hao Huang,Teng Qiu
The implementation of plasmonic materials in heterogeneous catalysis was limited due to the lack of experimental access in managing the plasmonic hot carriers. Herein, we propose a liquid-state surface-enhanced Raman scattering (SERS) technique to manipulate and visualize heterogeneous photocatalysis with transparent plasmonic chips. The liquid-state measurement conquers the difficulties that arise from the plasmon-induced thermal effects, and thus the plasmon based strategies can be extended to investigate a wider range of catalytic reactions. We demonstrated the selection of reaction products by modulating the plasmonic hot carriers and explored the mechanisms in several typical C–C coupling reactions with 4-bromothiophenol (4-BTP) as reactants. The real-time experimental results suggest brand new mechanisms of the formation of C–C bonds on plasmonic metal nanoparticles (NPs): the residue of 4-BTP, but not thiophenol (TP), is responsible for the C–C coupling. Furthermore, this technique was extended to study the evolution of the Suzuki–Miyaura reaction on nonplasmonic palladium metals by establishing the charge transfer channels between palladium and Au NPs. The cleavage and formation of chemical bonds in each individual reaction step were discerned, and the corresponding working mechanisms were clarified.
研究领域:
催化化学
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材料科学
·
光化学
✓ 已验证
DOI
高影响因子
APPLIED COMPOSITE MATERIALS
·
2022
·Vol. 29
·期 6
·2147-2163
·
IF 2.368
Wang Pei,Guo Yonggang,Du Sanming,Jia Yunchao,Zhang Hongbo,Yin Jian
Taking the advantages of porous ceramic (C/C-SiC composite) and transpiration cooling (Copper alloy), C/C-SiC-Cu composite was fabricated to attain a novel anti-ablation material for high temperature structure application of aerospace systems, via chemical vapor deposition and infiltration technologies. The effects of SiC content on microstructure, thermal conductivity, mechanical and ablation properties of C/C-SiC-Cu composite were investigated. As the SiC content increases from 0 vol% to 25.12 vol%, thermal conductivity, flexural strength and ablation resistance are improved by 84.99%, 78.76% and 53.68%, respectively. Thermal conductivity and thermal diffusivity exhibit proportional linear correlation with SiC content. The high SiC content could shorten the yield stage and increase the breaking strength during the flexural fracture process. When the SiC content is 25.12 vol%, the formation continuous and compact anti-ablation (SiO 2 ) layer is formed by oxidizing and melting fluidity processes during oxyacetylene ablation test, and the protective layer covers the ablation surface and slows down the oxidative ablation, which combines with the transpiration cooling effect of copper alloy to further improve ablation resistance of C/C-SiC-Cu composite.
研究领域:
航空航天材料科学
·
高温结构材料
✓ 已验证
DOI
高影响因子
APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
·
2024
·Vol. 130
·期 4
·1-14
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IF 2.5
Guo Chenxi,Yang Xin,Zhang Xiaxiang,Li Hongtao,Liao Mingdong,Huang Qizhong
To shorten the manufacturing process and enhance the ZrC content, C/C-SiC-ZrC composites were prepared using the nano-filler slurry infiltration method in combination with precursor infiltration and pyrolysis method. The effect of ZrC filler sizes on densification, microstructure, and properties of composites was studied. Results revealed that the ZrC content and density of the C/C-SiC-ZrC composites are inversely correlated to the filler size. The composites with nano-fillers reach the highest density of 2.67 g cm −3 as well as the lowest open porosity of 1.21%. After being ablated under oxyacetylene flame for 60 s, the composites with nano-fillers owns the lowest linear ablation rate and surface temperature, with 10 μms −1 and 2700 °C. Due to the highest ZrC content and best film-forming ability of nano-fillers, ZrO 2 outer layer with the densest structure can provide an enhanced protective effect, and the thickness of the oxide layer decreases from 509 to 264 μm as compared with micron fillers. Therefore, the oxidation damage of the composites is reduced, and the thickness of the SiC depletion layer decreases simultaneously. The above results further demonstrate that introducing ZrC nano-filler to the C/C-SiC-ZrC composites can considerably improve their ablative properties at 2700 °C.
研究领域:
材料科学
·
纳米技术
✓ 已验证
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Wang Shifu,Li Fuhua,Zhao Jian,Zeng Yaqiong,Li Yifan,Lin Zih-Yi,Lee Tsung-Ju,Liu Shuhui,Ren Xinyi,Wang Weijue,Chen Yusen,Hung Sung-Fu,Lu Ying-Rui,Cui Yi,Yang Xiaofeng,Li Xuning,Huang Yanqiang,Liu Bin
Manipulation C-C coupling pathway is of great importance for selective CO 2 electroreduction but remain challenging. Herein, two model Cu-based catalysts, by modifying Cu nanowires with Ag nanoparticles (AgCu NW) and Ag single atoms (Ag 1 Cu NW), respectively, are rationally designed for exploring the C-C coupling mechanisms in electrochemical CO 2 reduction reaction (CO 2 RR). Compared to AgCu NW, the Ag 1 Cu NW exhibits a more than 10-fold increase of C 2 selectivity in CO 2 reduction to ethanol, with ethanol-to-ethylene ratio increased from 0.41 over AgCu NW to 4.26 over Ag 1 Cu NW. Via a variety of o perando /in-situ techniques and theoretical calculation, the enhanced ethanol selectivity over Ag 1 Cu NW is attributed to the promoted H 2 O dissociation over the atomically dispersed Ag sites, which effectively accelerated *CO hydrogenation to form *CHO intermediate and facilitated asymmetric *CO-*CHO coupling over paired Cu atoms adjacent to single Ag atoms. Results of this work provide deep insight into the C-C coupling pathways towards target C 2+ product and shed light on the rational design of efficient CO 2 RR catalysts with paired active sites.
研究领域:
材料科学
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电化学
·
催化反应
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysts
·
2025
·Vol. 15
·期 3
·258
·
IF 4
Ling Xie,Zilong Huang,Yapeng Zhan,Jiahao Huang,Chao Wang,Riyang Shu,Junyao Wang,Libin Lei,Jianping Liu,Zhipeng Tian,Ying Chen
Cleavage of C-C bonds is crucial for hydrogen production via aqueous phase reforming of biomass-derived oxygenates. In this study, the hydrogen production performance and C-C bond cleavage capacity of Ni-W/AC catalysts with varying W/Ni ratios are evaluated using ethylene glycol as a model compound. A series of APR experiments conducted suggests that Ni-0.2W/AC catalyst exhibits the highest C1/C2+ratio of 15.87 and achieves a hydrogen yield of 47.76%. The enhanced Ni-W bimetallic interactions, which significantly improve the efficiency of C-C bond cleavage and increase catalyst activity by promoting active site dispersion, are confirmed by detailed characterization techniques. Further analysis of product distribution provides insights into the reaction pathways of ethylene glycol and the reaction mechanism for ethanol during aqueous phase reforming. All the results indicate that this catalytic reforming method effectively facilitates C-C bond cleavage and hydrogen production, contributing to a better understanding of APR mechanisms for biomass-derived oxygenates.
研究领域:
催化化学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2014
·
IF 3.309
Junjie Zhang,Fang Lu,Weiqiang Yu,Jiazhi Chen,Shuai Chen,Jin Gao,Jie Xu
The use of high pressure fossil derived hydrogen limits the commercial prospects of transforming sorbitol to glycols. Ni–Re/C catalyst which was developed in this study demonstrated high selectivity toward hydrogenative cleavage of C2–C3 and C3–C4 bonds of sorbitol to produce glycols under 1 MPa nitrogen. Acetol which is proposed as important intermediate to explain the reaction mechanism was first detected in the sorbitol conversion reactions. Detailed investigations showed that the presence of Re could prevent the sintering of Ni particles during the reduction process and make the catalyst efficiently generate hydrogen on the active sites to selectively cleave C–C bonds in sorbitol under nitrogen atmosphere.
研究领域:
催化化学
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 38
·32202-32211
·
IF 3.289
Changyan Wu,Xinwen Peng,Linxin Zhong,Xuehui Li,Runcang Sun
Catalytic process is the key process for many chemical industries. In this study, a novel heterogeneous Pd (CMH–Pd(0)) has been prepared by the deposition of palladium nanoparticles (Pd NPs) onto the surface of carboxymethyl functionalized hemicelluloses using ethanol as solvent and in situ reducing agent. The as prepared catalyst was characterized by TEM, HR-TEM, XRD, FT-IR, TGA and XPS. The loading level of Pd in the CMH–Pd(0) catalyst was 0.38 mmol g−1. The catalyst showed high catalytic activity and versatility towards Heck coupling reactions under aerobic conditions and could be readily recovered and reused in at least five successive cycles without obvious loss in activity. The catalyst is promising for its renewability, environmental benefits, efficient catalytic activity, mild reaction conditions, simple product work-up and easy catalyst recovery.
研究领域:
化学工程
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 117
·96372-96376
·
IF 3.84
Zheng-Jun Wang,Peng-Hui Wang,Jing-Jing Lv,Jiu-Ju Feng,Xinhua Xu,Ai-Jun Wang,Chak-Tong Au,Renhua Qiu
Commercial copolymer Luviset clear (L1), an environmentally benign and efficient ligand, was used to facilitate the catalytic performance of Cu(NO3)2 for homo-coupling of terminal alkynes. A series of substituted aromatic and aliphatic terminal alkynes were investigated. It was found that Cu(NO3)2@L1 can catalyze the C–C coupling reactions without any other base, and the corresponding diynes are generated in good to excellent yield. X-ray photoelectron spectroscopy was used to study the reaction mechanism, and the results evidence a Cu(II)/Cu(I) catalytic system. Additionally, the catalyst can be easily separated and reused without showing significant loss of catalytic activity.
研究领域:
化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Yanyan Wang,Yu Liu,Jiyang Li,Yuanyuan Liu,Weiqiang Zhang,Mingming Yang,Yajun Jian,Ping Zuo,Ziwei Gao
The position of Pd species in/on zeolites is crucial for the activity of metal/metal oxide catalysts. It is still a challenge to highly disperse and stabilize the metal species on zeolites and shorten diffusion paths to maintain high catalytic activity. Here, we report an effective strategy for preparing highly efficient zeolite-supported Pd(II) catalysts by positioning Pd(II) species on the surface of a zeolite with an anion framework based on the principle of charge balance. The catalyst was prepared in situ in a C–C cross-coupling reaction. Due to the change in the metal–support interaction, Pd species have migrated from the inside to the surface of the zeolite, which shortens the diffusion path of reactants and thus ensures the high activity of the catalyst. Pd species exhibit aggregation resistance in alkaline systems and tend to be confined in the traps with high charge density. Compared to unactivated Pd@USY, the efficiency of the activated catalysts has at least doubled in catalyzing the Sonogashira and Suzuki–Miyaura reactions. This study represents a new activation approach for zeolite-supported Pd catalysts, which may help to design efficient catalysts.
研究领域:
催化化学
·
材料化学
·
有机合成
·
纳米催化
·
多相催化
✓ 已验证
DOI
高影响因子
Surfaces and Interfaces
·
2025
·
IF 6.3
Ting Li,Jiantao Bi,Huajing Li,Qing Li,Yuangang Li
The synergistic coupling of photocatalytic C C bond construction and H 2 evolution presents a promising strategy for concurrent organic synthesis and sustainable H 2 evolution. Nevertheless, precisely regulating the reaction pathways to enhance the selectivity of target products remains a challenging. Here, the Sv-CdS/TiO 2 Ni 2 P photocatalyst containing sulfur vacancies was synthesized via calcination, achieving highly selective conversion of 4-pyridinemethanol into the C C coupling product 1,2-di-(4-pyridyl)-1,2-ethanediol under visible-light irradiation, with a selectivity of 96.59 %. In comparison, the M-CdS/TiO 2 Ni 2 P photocatalyst prepared by mechanical mixing exhibits superior H 2 evolution activity of 6.48 mmol·g -1 ·h -1 . Mechanism studies reveal that 4-pyridinemethanol interacts with the Sv-CdS/TiO 2 Ni 2 P photocatalyst through the N atom, which preferentially activates the sp 3 C H bond of 4-pyridinemethanol to generate •CH(OH)C 5 H 4 N radical for further C C coupling reaction. This work not only highlights the selective regulation of the 4-pyridinemethanol C C coupling pathway by sulfur vacancies engineering, but also provides new insights for achieving efficient photocatalytic organic synthesis and green H 2 evolution.
研究领域:
光催化
·
有机合成
·
材料科学
·
环境化学
·
能量转换
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2025
·
IF 6.2
Yuanming Zhou,Shuxin Li,Shuangxing Zhu,Ruizhi Liu,Zhenxiao Tang,Maozhong Yi,Ke Peng
To investigate the influence of (Ta,Zr)C on the ablation resistance of C/C composites, C/C-(Ta 0.5 Zr 0.5 )C-SiC, C/C-(Ta 0.33 Zr 0.67 )C-SiC, and C/C-(Ta 0.2 Zr 0.8 )C-SiC were prepared with different Zr/Ta ratios through high-solid-loading slurry impregnation combined with precursor infiltration and pyrolysis. The flexural performance and ablation resistance both improved with an increasing Zr/Ta ratio. Compared to C/C-(Ta 0.5 Zr 0.5 )C-SiC and C/C-(Ta 0.33 Zr 0.67 )C-SiC, the flexural strength of C/C-(Ta 0.2 Zr 0.8 )C-SiC increased by 74.17 % and 24.29 %, respectively. The mass ablation rate was reduced by 74.33 % and 81.02 %, while the linear ablation rate was reduced by 98.60 % and 97.65 % after 120 s of ablation, respectively. The variations in Zr/Ta ratios affected the formation, integrity, and performance of the microstructure, which was composed of a Zr-rich oxide skeleton combined with Ta-rich oxide binder within the Ta-Zr-O oxide layer on the composite surface, ultimately enhancing the overall ablation resistance of these composites.
研究领域:
材料科学
·
航空航天工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Zongyi Huang,Pengfei Sun,Huizhen Zhang,Haikun Zhang,Shuhong Zhang,Zhou Chen,Xiaodong Yi,Shunji Xie
The integration of solar-driven H2 evolution with the selective conversion of biomass-derived alcohols into value-added chemicals has gained significant attention for full use of electrons and holes. We develop a dual-functional photocatalyst for highly selective oxidation of the Cα–H bond of benzyl alcohol to C–C coupled products (hydrobenzoin and deoxybenzoin), in cooperation with H2 evolution, using point-to-face interface engineering by decorating CdS quantum dots on Zn2In2S5 nanosheets (CdS QDs/Zn2In2S5 NS). The CdS QDs/Zn2In2S5 NS exhibit a high H2 evolution rate of 13 mmol g–1 h–1 and C–C coupled products formation rate of 10.8 mmol g–1 h–1 with 96.3% selectivity. Benzyl alcohol conversion achieves 91% with an 89% yield of C–C coupled products in gram-scale. The introduction of CdS enhances the interfacial contact, facilitating the efficient spatial separation of photogenerated electron–hole pairs and providing active sites for H2 evolution. In situ characterization and DFT calculation reveal that the carbon-centered radical •CH(OH)C6H5, generated by abstracting the Cα–H bond of benzyl alcohol, is the reactive intermediate in the photocatalytic C–C coupled process.
研究领域:
化学工程
·
材料科学
·
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）