ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Yuanyuan An,Guoxiu Hao,Xinyue Wang,Li Zhou,Mengyao Wu,Jialong Ma,Lien-Yang Chou
In this study, we synthesized CeO2 possessing an open pore structure and verified its structural differences compared to CeO2 lacking such an open pore structure. Using these two CeO2 samples as catalyst supports and loading them with Pd metals, a series of characterizations were carried out on the resultant catalysts to analyze their structures and properties meticulously. We have elucidated the influence of the open pore structure on the loading position of Pd. Hydrogenation reactions involving alkynes and alkenes were employed to confirm the existence of steric hindrance effects caused by the pore structure differences. Furthermore, we applied these catalysts to more valuable industrial reaction systems, demonstrating that the unique pore structures of directly synthesized CeO2 can also exhibit excellent performance in practical applications.
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
Catalysis Science & Technology
·
2018
·Vol. 8
·期 24
·6384-6395
·
IF 5.365
Zhiyang Zhang,Yanle Li,Jing Gu,Liping Ding,Nianhua Xue,Luming Peng,Xuefeng Guo,Yan Zhu,Jing Ma,Weiping Ding
The electrostatic field of a dielectric cavity is powerful for modulating many aspects of confined metal clusters. Here we report that the catalytic properties of Ptn clusters confined in X-zeolite cages are strongly tuned by altering the zeolitic field, which is achieved by using different cations (Na+, Cs+, Ca2+ or La3+) to balance the negative framework of the zeolite. Compared with Ptn@LaX, for example, Ptn@CsX shows a surprising ∼5500% enhancement in TOF value for phenol hydrogenation to cyclohexanol. Electrostatic field modulation leads to gradual changes of electronic properties such as the Fermi levels/d-band centers of the Ptn clusters, as revealed by DFT calculations and experimental characterizations. The decreases in Fermi levels of the Ptn clusters benefit the hydrogenation of –CCH groups (phenylacetylene and acetylene) and –NO2 groups (nitrobenzene, o-nitroanisole and o-chloronitrobenzene) but are detrimental for aromatic ring hydrogenation (phenol). These findings are important for the design of high performance catalysts.
研究领域:
化学
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材料科学
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DOI
高影响因子
Nanoscale
·
2018
·Vol. 10
·期 47
·22348-22356
·
IF 7.233
Xusheng Cheng,Dongxu Wang,Jiancong Liu,Xin Kang,Haijing Yan,Aiping Wu,Ying Gu,Chungui Tian,Honggang Fu
Decreasing Pd usage whilst maintaining a superior performance is promising, but remains a challenge in the catalytic field. Herein, we have demonstrated the highly efficient promotion of Mo2N with a reduced amount of Pd for the liquid-phase hydrogenation reaction. The Mo2N (2–3 nm) was uniformly anchored onto mesoporous SBA-15 by using PMo12 as the Mo source. The small size and good dispersion of Mo2N is favourable for allowing their effective contact with post-loading Pd. This good contact is conducive to developing a synergistic catalyst, which was verified by studying the liquid-phase hydrogenation of p-nitrophenol (PNP) to p-aminophenol (PAP) with NaBH4 as the H source. The conversion ability of PNP to PAP on 1 wt% Pd–Mo2N/SBA-15 was vastly superior to 1 wt% Pd/SBA-15 and even better than 20 wt% Pd/SBA-15. The low-Pd, highly efficient catalysis is ascribed to the transfer of the electrons from Mo2N to Pd for the easy activation of H. The synergy can be affected by the type of support used. SBA-15 is superior to SiO2 and the other supports, which could be related to the large surface area and the plentiful number of pores on SBA-15, which is favourable to the dispersion of Pd and Mo2N, and the transfer/diffusion of the reactants. In particular, a highly efficient catalyst can be achieved at an even more reduced Pd loading (0.05 wt%). The current method describes the design of a highly efficient catalyst for the hydrogenation reaction using low amounts of noble metals.
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
PubMed
高影响因子
GREEN CHEMISTRY
·
2017
·Vol. 19
·期 21
·5103-5113
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IF 9.125
Ying Duan,Min Zheng,Dongmi Li,Dongsheng Deng,Lu-Fang Ma,Yanliang Yang
The catalytic conversion of HMF to 2-hydroxy-3-methyl-2-cyclopenten-1-one (MCP), which is a valuable edible essence that has traditionally been obtained from adipic acid, was achieved with an isolated yield of 58%. This procedure comprised two steps: the hydrogenation of 5-hydroxymethylfurfural (HMF) to 1-hydroxy-2,5-hexanedione (HHD) in water on Pd/Nb2O5 catalysts and then the isomerization of HHD to MCP in the presence of a base. The Nb2O5 supports, which were acidic, were characterized by FTIR, XRD and NH3-TPD. The supported Pd/Nb2O5 catalysts, in which Pd was highly dispersed, were synthesized employing cyclohexene as a reductant and were characterized by XRD, TEM, ICP-AES, XPS, EDX and CO pulse chemisorption. The high conversion of HMF was attributed to the high dispersion of Pd, and the acidity of the supports led to high selectivity for HHD. The conversion of HHD to MCP was an intramolecular aldol condensation reaction, and the protonic solvent favored this reaction. Ca–Al was proved to be an effective solid base for the conversion of HHD to MCP in water.
研究领域:
化学工程
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催化化学
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产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Zidan Zou,Chun Chen,Zhi Hu,Yue Shen,Zhen Fu,Wenchao Li,Yunxia Zhang,Haimin Zhang,Huijun Zhao,Guozhong Wang
Silica is one of the most referenced materials for the preparation of heterogeneous metal catalysts. However, silica spheres with smooth surfaces have difficulty encapsulating active metals due to their small surface area and the presence of only a handful of silicon hydroxyl groups on the surface. In this work, the silica sphere has been first consciously transformed into a hierarchical SiO 2 @silicate structure, and then the core–shell hetero-structured SiO 2 @Ni/SiO 2 catalyst can be tactfully obtained by reducing treatment. The core–shell catalyst is composed of a rigid core (SiO 2 ) and a rough shell (Ni NPs highly disperse on nanosheet SiO 2 ), which are carefully verified by X-ray diffraction (XRD), transmission electron microscope (TEM), field scanning electron microscope (FESEM), H 2 -TPR/TPD and X-ray photoelectron spectroscopy (XPS). The derived SiO 2 @Ni/SiO 2 catalyst can selectively hydrogenate vanillin in the aqueous phase at near-room temperature (40 ℃) and low hydrogen pressure (2 MPa H 2 ), and the conversion of vanillin can be up to 99%. The preparation method of the SiO 2 @Ni/SiO 2 catalyst is simple and can be amplified to a large scale at a low price, thus can be adopted to convert bio-derived unsaturated compounds in an economical and eco-friendly way.
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
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Hairus Abdullah,Yu-Rou Ko,Dong-Hau Kuo,Noto Susanto Gultom
La–Sn-codoped Zn(O,S) catalysts were synthesized with different amounts (0%, 2.5%, 5%, and 10%) of Sn and a constant amount (10%) of La to improve the photocatalytic hydrogenation reaction (PHR) of azobenzene to aniline. The as-prepared catalysts were carefully characterized and tested for a hydrogenation reaction. The incorporation of Sn significantly enhanced the PHR activities since the incorporated Sn in the Zn(O,S) lattices could increase the conductivity of the catalysts to improve the charge transfer during the catalytic reaction as indicated with EIS measurement. Further measurement with a photoresponse of La–Sn-codoped Zn(O,S) catalysts also exhibited relatively higher intensities as compared to those of La-doped Zn(O,S) and Sn-doped Zn(O,S) catalysts. On the basis of the measurement results of EIS and transient photo current, the La–Sn-codoped Zn(O,S) with the best properties was further utilized for PHR to convert azobenzene to aniline. GC–MS measurement confirmed that 15 ppm azobenzene could be totally converted to aniline in only 60 min which was achieved with a catalyst that was prepared with 5%-Sn and 10%-La doping. The relatively short reaction time indicated that the as-prepared catalyst had a strong reduction capability able to cleave the strong bonding of N═N in azobenzene. The reaction kinetic of the N═N bond cleavage was elucidated based on solvation, adsorption, pinning, and photocatalytic hydrogenation processes on the catalyst surfaces.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
GREEN CHEMISTRY
·
2023
·Vol. 25
·期 5
·1823-1834
·
IF 9.8
Ying Duan,Chi Zhang,Dongsheng Deng,Dong Sui,Xiaohan Gao,Yanliang Yang
The rearrangement of furan rings for valuable chemicals is an important topic for biomass conversion. In this study, 2,5-di(hydroxymethyl)furan (BHMF) was selectively converted to 6-methyldihydro-2H-pyran-3(4H)-one (MDPO) and 1-hydroxy-2,5-hexanedione (HHD) under atmospheric H2 pressure in water. The selectivity to MDPO or HHD could be regulated by a catalyst. The parameters (temperature, pH, catalyst loading, and BHMF concentration) for the transformation of BHMF were studied. The selectivity for the transformation of BHMF was very sensitive to the reaction conditions, especially for the conversion of BHMF to MDPO. 68% selectivity to MDPO on Pd/C and 72% selectivity to HHD on Rh/C were achieved under the optimized conditions. Both Pd/C and Rh/C could be reused at least 5 times without the loss of activity. The fresh and used Pd/C and Rh/C were characterized by XRD, XPS, SEM, TEM, EDS mappings and ICP-OES to study the changes during the reaction. The reaction process was studied through controlled experiments, and 6-methylene-2H-pyran-3(6H)-one (MEPO) and 6-hydroxy-6-methyl-2H-pyran-3(6H)-one (HMPO) were identified as intermediates. A reasonable reaction mechanism was proposed and the different selectivity to MDPO and HHD was well explained based on the controlled experiments and DFT calculations. The conditional sensitivity for the selectivity to MDPO and HHD could also be interpreted by the proposed reaction pathway.
研究领域:
化学工程
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生物质能
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催化科学
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产品关联
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Wang Zhe,Wang Chunpeng,Mao Shanjun,Lu Bing,Chen Yuzhuo,Zhang Xie,Chen Zhirong,Wang Yong
Decoupling the electronic and geometric effects has been a long cherished goal for heterogeneous catalysis due to their tangled relationship. Here, a novel orthogonal decomposition method is firstly proposed to settle this issue in p -chloronitrobenzene hydrogenation reaction on size- and shape-controlled Pt nanoparticles (NPs) carried on various supports. Results suggest Fermi levels of catalysts can be modulated by supports with varied work function ( W f ). And the selectivity on Pt NPs of similar size and shape is linearly related with the W f of support. Optimized Fermi levels of the catalysts with large W f weaken the ability of Pt NPs to fill valence electrons into the antibonding orbital of C–Cl bond, finally suppressing the hydrodehalogenation side reaction. Foremost, the geometric effect is firstly spun off through orthogonal relation based on series of linear relationships over various sizes of Pt NPs reflecting the electronic effect. Moreover, separable nested double coordinate system is established to quantitatively evaluate the two effects.
研究领域:
催化
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化学工程
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2024
·Vol. 35
·期 11
·1-17
·
IF 2.8
Pan Deng,Wang Yanan,Lin Liwei,Zhang Yuzhe,Zhou Man,Li Zhongyu,Xu Song
Photothermal catalytic CO 2 reduction can combine photocatalysis and thermal catalysis by using full-spectrum solar energy to convert CO 2 into high value-added chemicals. This can effectively alleviate the problems of excessive CO 2 emissions and thermal catalytic energy waste. In this paper, a novel catalyst was prepared using Ce-MOF as a precursor to generate Cu/Ni/CeO 2 for efficient reduction of CO 2 to CO by hydrogenation. Due to the rod-like structure of CeO 2 and the high dispersion of Cu and Ni nanoparticles, 10%Cu 5%Ni CeO 2 can achieve a catalytic activity of 54.21 mmol g −1 h −1 in the full solar spectrum. The supported Cu and Ni metals are the active sites for catalytic reduction. Meanwhile, Cu and Ni enhanced the light absorption ability of the catalyst and the surface temperature under illumination. This is due to the hot charge carriers generated by LSPR effect in Ni and Cu metal nanoparticles, which can dissipate energy through local heating, thus increasing the temperature of the catalyst under illumination. It can be found that the CO 2 reduction activity of photo-assisted thermocatalysis is higher than that of thermal catalysis under the same conditions. Therefore, the combined effect of the electrons generated by UV–Vis light and the heating effect of near-infrared light on catalyst could improve the catalytic activity. This work might provide a potential strategy for efficient photothermal reduction of CO 2 in the future.
研究领域:
化学工程
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环境科学
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材料科学
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2024
·
IF 2.3
Liang Yongjia,Zuo Jianliang,Cai Zhaohao,Lin Jing,Liu Zili
The direct conversion of furfural (FA) from biomass to pentanediols (PeDs), including 1,2-PeD and 1,5-PeD, is important for replacing fossil resources and developing bio-based polyesters from renewable sources. However, achieving high selectivity for the C–O hydrogenation of the furan ring remains a significant challenge. In this study, we synthesized a series of trimetallic CuCoLa catalysts, using a coprecipitation method with various metal ratios. The reduced CuCoLa catalyst with a metal ratio of 1/3/1, exhibited the highest activity for the selective hydrogenolysis of FA to PeDs. Under optimal reaction conditions (160 °C, 4 MPa H 2 for 9 h), CuCoLa(1/3/1)-R achieved yields of 21.7% for 1,2-PeD and 50.1% for 1,5-PeD. Furthermore, the catalyst remained stable after five cycles of FA conversion to PeDs. The high selectivity for PeDs is attributed to the synergistic interaction between Cu and Co and the appropriate number of basic surface sites. Graphical Abstract
研究领域:
催化化学
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可再生资源化学
·
生物质转化
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2021
·Vol. 23
·期 18
·7065-7073
·
IF 10.182
Liang Jiang,Guangyue Xu,Yao Fu
The conversion of levulinic acid (LA) to γ-valerolactone (GVL) is one of the most important reactions from biomass-derived platform chemicals to value-added chemicals. In this work, nitrogen-doped carbon was introduced into a Ni/Al2O3 catalyst and was employed for the hydrogenation of LA to GVL with a full conversion and equivalent yield under mild conditions, at as low as ambient hydrogen pressure and 130 °C for 6 h. The doping of nitrogen introduced NiNx species and the imperfection of modified nitrogen-doped carbon were beneficial for the selective hydrogenation of carbonyl groups. This catalyst showed excellent activity and selectivity in various solvents and could be recycled for at least 6 runs with little deactivation. In addition to LA, various substrates with both carbonyl and carboxyl groups could also be selectively hydrogenated to the corresponding lactones. This study offers both theoretical foundation and practical instructions for the high-efficiency conversion of LA to GVL over non-noble metal catalysts under mild conditions, especially ambient H2 pressure.
研究领域:
催化化学
·
生物质能转化
✓ 已验证
DOI
高影响因子
Journal of Chemistry
·
2020
·
IF 1.79
Zhaozhuo Yu,Weibo Wu,Hu Li,Song Yang
Hydrogenation of bio-based furfural (FUR) to furfuryl alcohol (FFA) is tremendously expanding the application of biomass in many industries such as resins, biofuels, and pharmaceuticals. However, mass manufacture of FFA from FUR is restrained by strict requirements of reaction conditions and expensive catalysts. In this work, an economical and benign catalytic system, containing an easily prepared and reusable catalyst 5 wt.% KF/ZrO2 and a low-cost hydrogen source polymethylhydrosiloxane (PMHS), was developed to be efficient for the hydrogenation of FUR to high-value FFA under mild conditions. The catalyst reactivity was found to be remarkably influenced by the support acid-base properties and KF loading doge. In the presence of 5 wt.% KF/ZrO2, a high FFA yield of 97% and FUR conversion of 99% could be obtained at 25°C in just 0.5 h, which was superior to those attained with other tested catalysts. The KF/ZrO2 catalyst could be recycled at least five times, with the FFA yield slightly decreasing from 97% to 71%. The spare decrease in FFA yield is possibly attributed to the catalyst pore blocking, as clarified by SEM, BET, XPS, and ICP-MS measurements of the fresh and reused catalysts.
研究领域:
化学工程
·
可再生资源利用
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）