CHINESE JOURNAL OF CATALYSIS
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2021
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IF 8.271
Weiyin Wang,Lu Lin,Haifeng Qi,Wenxiu Cao,Zhi Li,Shaohua Chen,Xiaoxuan Zou,Tiehong Chen,Nanfang Tang,Weiyu Song,Aiqin Wang,Wenhao Luo
The catalytic hydrogenation of halonitroarenes to haloanilines is a green and sustainable process for the production of key nitrogen-containing intermediates in fine chemical industry. Chemoselective hydrogenation poses a significant challenge, which requires the rational design of the catalysts with proper hydrogenation ability for nitro group and simultaneously preventing dehalogenation of halogen group. Herein, a highly effective Rh@Al 2 O 3 @C single-atom catalyst (SAC) was developed for the hydrogenation of m -chloronitrobenzene ( m -CNB) to m -chloroaniline ( m -CAN), through an in-situ grafting of metal during the assembly of MIL-53 (Al), followed by confined pyrolysis . Extensive characterizations reveal an exquisite structure of the Rh@Al 2 O 3 @C, containing atomically dispersed Rh sites onto Al 2 O 3 confined by the amorphous carbon. The five-coordinated aluminum (Al V ) species are essential for achieving the atomic dispersion of Rh atoms, providing the unsaturated coordinative sites for metal. Compared to the benchmark Rh/γ-Al 2 O 3 and Rh/C nanocatalysts, the Rh@Al 2 O 3 @C SAC affords an excellent turnover frequency of 2317 mol m -CNB ·mol Rh –1 ·h –1 , the highest value to date in heterogeneous catalyst systems for the hydrogenation of m -CNB at 313 K and 20 bar H 2 , together with a sustained selectivity to m -CAN (~98%) during five consecutive runs. The superior catalytic performance of the Rh@Al 2 O 3 @C is attributed to a proper modulation of electronic structure of hydrogenation metal by forming SAC, together with an enhanced accessibility of acid function sites.
研究领域:
催化化学
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材料科学
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精细化工
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产品关联
DOI
高影响因子
FUEL
·
2025
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IF 7.5
Geng Chen,Zexiang Bi,Xu Li,Jinxiang Dong
The industrial utilisation of Fischer–Tropsch synthesis (FTS) products, particularly the valuable C5–C9 linear α-olefins, has been hindered by the high energy-intensive separation of olefins and alkanes with identical carbon numbers. This study presents a comprehensive process integrating the selective dimerisation of linear α-olefins to α-olefin dimers, enabling their separation from paraffins in FTS products. These dimers are subsequently converted into branched-chain aldehyde intermediates through heterogeneous hydroformylation using Rh/C as the catalyst. Notably, optimising the reaction conditions achieved the main product aldehyde of α-olefin dimers with excellent selectivity (up to 86.66 %) at 65 °C, compared to linear α-olefins, which exhibited only 49.31 % selectivity. In-situ IR spectroscopy was used to monitor the entire reaction process. The resulting branched aldehyde intermediates were further transformed into branched acids or branched alcohols through oxidation or reduction reactions, respectively. These products have diverse applications as surfactants, coal flotation agents, and cutting fluid additives. The synthesised compounds were characterised using FT-IR, GC, GC–MS, and NMR. In addition, a comprehensive evaluation of their physicochemical properties was conducted. This study provides a versatile design strategy for developing high-value intermediates from α-olefins in the FTS.
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
ENERGY & FUELS
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2022
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IF 4.654
Xiuhong Zhang,Dong Wang,Xiao Chen,Longwei Meng,Changhai Liang
The hydrogenation of polycyclic aromatic hydrocarbons (PAHs) over highly efficient and stable catalysts to fine chemicals and intermediates for producing chemical materials is an effective approach to realize the high value-added utilization of coal tar and slurry oil. Herein, two kinds of Al2O3-supported Pt and Rh catalysts are synthesized by strong electrostatic adsorption (SEA) and used to catalyze the hydrogenation of anthracene. Compared with the traditional catalysts synthesized by wet impregnation, the Pt/Al2O3-SEA and Rh/Al2O3-SEA catalysts have smaller active metal particle sizes and higher dispersion, which can expose more active centers, showing higher catalytic activity. Interestingly, anthracene may be preferentially adsorbed on the surface of the Pt/Al2O3 catalyst in a parallel manner but on the surface of the Rh/Al2O3 catalyst in a lateral manner, which leads to the different hydrogenation routes. 9,10-Dihydroanthracene is an initial product for the hydrogenation of anthracene, which is rearranged into tetrahydroanthracene and subsequently hydrogenated to symmetrical octahydroanthracene (sym-OHA) over the Pt/Al2O3 catalyst. The high selectivity to sym-OHA (93%) with the conversion of anthracene near 100% can be achieved in the hydrogenation of anthracene at 240 °C and 7 MPa for 10 h. Additionally, due to the strong anchoring effect, the Pt/Al2O3-SEA catalyst shows high stability for six cycles. This work supplies a new tactic to develop high-performance catalysts for selective hydrogenation of PAHs to important monomers for synthesizing chemical materials.
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
ACTA PHYSICO-CHIMICA SINICA
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2017
·Vol. 33
·期 9
·1865-1874
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IF 0.767
NING Hong-Yan,YANG Qi-Lei,YANG Xiao,LI Ying-Xia,SONG Zhao-Yu,LU Yi-Ren,ZHANG Li-Hong,LIU Yuan
Rh-Mn-based catalysts are promising for ethanol synthesis from syngas. In this work, a carbon fiber (CF)-supported Rh-Mn catalyst, with highly dispersed Rh and close contact Rh-Mn species, has been prepared by a new in situ polymerization route using citric acid and ethylene
glycol interaction. The structure and physicochemical properties of both the calcined and reduced samples have been characterized by TPR, XRD, TEM, EDS, CO-TPD, H2 chemisorption, and XPS techniques and the catalytic performance for ethanol synthesis from syngas has been evaluated.
The results show that the new method is beneficial in forming close contact Rh-Mn species than that obtained with the conventional impregnation method. This can enhance the dispersion and sintering resistance of Rh and effectively improve the activity of CO hydrogenation and the selectivity
to ethanol in ethanol synthesis from syngas.
研究领域:
化学工程
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材料科学
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催化化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2016
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IF 3.205
Jianmin Chen,Qilu Yao,Jia Zhu,Xiangshu Chen,Zhang-Hui Lu
Bimetallic Rh–Ni nanoparticles (NPs) immobilized on the cerium hydroxide carbonate (Ce(OH)CO 3 ) have been successfully prepared by a facile co-reduction route, and characterized by XRD , SEM , TEM , EDX, ICP , XPS , and TG-DTA. The as-synthesized Rh–Ni/Ce(OH)CO 3 nanocomposites (NCs) with different metal compositions were applied as the highly efficient catalysts for hydrogen generation from the alkaline solution of hydrazine (N 2 H 4 ). Especially, the Rh 55 Ni 45 /Ce(OH)CO 3 NCs exerted the highly activity and 100% H 2 selectivity for the decomposition of hydrazine, providing high turnover frequency (TOF) values of 150 h −1 at 30 °C and 395 h −1 at 50 °C, respectively, relative high values for the metal catalysts . The activation energy for the decomposition of hydrazine catalyzed by Rh 55 Ni 45 /Ce(OH)CO 3 NCs was measured to be 38.8 kJ/mol, lower than most of the values reported for this reaction using many different catalysts. This excellent catalytic performance could be attributed to not only the strain and ligand effects between Rh and Ni, but also the strong interaction between RhNi NPs and Ce(OH)CO 3 support. Such a highly catalyst may greatly encourage the practical application of hydrazine as a hydrogen storage material.
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
TRANSFUSION MEDICINE
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2021
·Vol. 31
·期 4
·277-285
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IF 2.019
Hongtian Chen,Piao Lv,Ziwei Liu,Wanjun Chen,Yuan Yao,Chixiang Liu,Qiong Cao,Huayou Zhou
Objectives The purpose of this study was to investigate the association and impact of TMEM50A on RH genes activity and function. Background SMP1 is located on chromosome 1p36.11 in the RH gene locus, between the RHD and RHCE gene, where its position may be linked to RH haplotypes and contribute to selective pressures regarding certain RH haplotypes. TMEM50A is encoded by the SMP1 located in the intergenic region of RH , its influence on the function of the RH genes remains unclear. Methods The expression of TMEM50A was regulated by transfection of plasmid and siRNA in K562 cell model. Western blot and real-time PCR were used to detect possible expression changes in the RH . The ammonium transport function of cells was monitored using pH-sensitive dye, while transcriptome sequencing was used to predict the potential function of TMEM50A. Results The overexpression of TMEM50A significantly up-regulated RHCE gene activity (63.56%). The inhibition of TMEM50A resulted in significantly decreased RHCE (41.82%) and RHD expression (27.35%). Compared to control group, there was no significant change in the NH 4 + transport function of cells in the overexpressed TMEM50A group. Transcriptome analysis showed that TMEM50A not only affected the transcription of target gene through splicing activities, but also played a role in the development of embryonic nervous system. Conclusions TMEM50A may regulate the expression of RH gene by affecting the stability of RH mRNA through splicing function. It speculates that TMEM50A may play an important role in the development of embryonic nervous system.
研究领域:
分子生物学
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遗传学
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细胞生物学
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转录组学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Wenjie Xue,Hongxia Liu,Baohua Mao,Honglei Liu,Minghuang Qiu,Chengguang Yang,Xinqing Chen,Yuhan Sun
Hydrogen is a promising candidate to replace the exhausting fossil fuels. However, it is still a big challenge for hydrogen storage. Liquid organic hydrogen carrier (LOHC), which possesses high safety and purity, easy transport and reversibility, is highly attractive for hydrogen storage. Herein we report a new reusable bimetallic Pd-Rh nanoparticles (NPs) catalyst with synergy effect, boosting both the hydrogenation of N-ethylcarbazole (NEC) and dehydrogenation of dodecahydro-N-ethylcarbazole (12H-NEC), which allows multiple cycles of reversible high-weight% hydrogen storage and uptake in short reaction time. Various ex- and in-situ characterizations evidenced that the superior activity was attributed to the bimetallic Pd-Rh NPs cluster structure on the surface of γ-Al 2 O 3 support. The mechanism of NEC hydrogenation over the Pd-Rh catalyst was proposed and verified by density functional theory (DFT) calculations. Such a strategy can be extended to other LOHCs and sheds light onto the development of LOHCs as energy vectors.
研究领域:
化学工程
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材料科学
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能源技术
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产品关联
DOI
高影响因子
ACS Applied Energy Materials
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2021
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IF 6.024
Lin-Chang Liu,Hong-Lin Zhu,Yue-Qing Zheng
Ammonia borane (NH3BH3, referred to as AB) hydrolytic dehydrogenation is regarded as a feasible strategy for hydrogen production owing to its high hydrogen content, pollution-free nature, and high stability. Metal nitrogen-doped carbon materials (M-N-C) are considered as an ideal candidate support of catalysts with AB hydrolytic dehydrogenation due to the advantages of low cost, large specific surface area, rich defective site, and good chemical stability. In this work, tubular Ni@Ni-N-C was successfully synthesized by high-temperature pyrolysis, and then, Rh nanoparticles were decorated on the support Ni@Ni-N-C by impregnation and reduction to prepare a series of Rh/Ni@Ni-N-C. The best catalytic performance of catalysts is obtained using Ni@Ni-N-C with an Rh loading of 0.74 wt %, showing a turnover frequency as high as 782.18 min–1 and an apparent activation energy (Ea) as low as 25.86 kJ mol–1, which could be attributed to the strong interaction between Rh and the defective site of the support.
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
Desalination and Water Treatment
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2016
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IF 1.272
Yili Ge,Ying Xiang,Yu He,Meiyan Ji,Gongwu Song
A versatile Zn-TiO2/RH/Fe3O4 ternary composite material on the basis of rice hull was prepared and characterized by X-ray diffraction, Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy, energy dispersive X-ray spectroscopy, and vibrating sample magnetometer analysis. Its ability to photocatalytically remove Rhodamine B (RhB) in wastewater was investigated in a photochemical reactor by means of ultraviolet and visible spectrophotometry and FT-IR. Research results show that the catalytic degradation rate of RhB from aqueous solution is close to 100% when using synthesized Zn-TiO2/RH/Fe3O4 as a catalyst under irradiation of visible light for 120 min. The as-prepared visible light-driven photocatalyst Zn-TiO2/RH/Fe3O4 material has high performance with excellent recyclability, magnetic separation feature, and photocatalysis activity in wastewater treatment.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2025
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IF 4.8
Xuying Bian,Hualiang An,Xinqiang Zhao,Yanji Wang
The selective hydrogenation of dimethyl toluene-2,4-dicarbamate (TDC) to methyl cyclohexyl-2,4-dicarbamate (HTDC) is an important process for non-phosgene synthesis of methylcyclohexane-2,4-diisocyanate (HTDI). We prepared Rh/γ-Al 2 O 3 catalysts with an Rh particle size of 1.8–6.7 nm and studied size effect on TDC selective hydrogenation. The results showed that the catalytic activities of Rh/γ-Al 2 O 3 increase monotonously with increasing Rh particle size. This demonstrated that Rh/γ-Al 2 O 3 catalyst dedicates a negative size effect or an antipathetic structure sensitivity. Based on the characterization, we found that the geometric property of Rh is the main factor affecting the activity of catalyst. Combined with the proposed Rh particle model, it was inferred that the Rh (111) plays a major role in the TDC selective hydrogenation and the terrace sites are beneficial to promote the adsorption of TDC. The study on size effect can provide a guidance for the design and preparation of highly efficient Rh-based catalysts for TDC selective hydrogenation.
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
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Lihua Zhu,Huaze Zhu,Mohsen Shakouri,Linghai Zeng,Zhiqing Yang,Yongfeng Hu,Hengqiang Ye,Hui Wang,Bing Hui Chen,Rafael Luque
Mono- and bimetallic nanoparticles (NPs) supported on carbon nanotubes (CNTs) (Ni/CNTs, Co/CNTs and NiCo/CNTs) were synthesized at room temperature (RT) via hydrazine hydrate reduction method without any surfactant. The galvanic replacement reaction was exploited to prepare Rh/Ni/CNTs, Rh/Co/CNTs and Rh/NiCo/CNTs supported nanocatalysts. Prepared nanocatalysts were extensively characterized using an array of advanced analytical techniques. The catalytic performance of the catalysts was evaluated in the hydrogenation of tetralin. Reduced Rh/NiCo/CNTs catalyst (Rh-on-NiCo NP) exhibited high catalytic activity at RT, significantly improved as compared to Rh/Ni/CNTs and Rh/Co/CNTs due to the interfacial nano-synergy effect among different metallic related species (Rh, Ni and Co). In-situ XAS results confirmed the mechanism of the interfacial nano-synergy effect, wherein Rh sites provided activated hydrogen species (H*), and H* was subsequently transferred to the surface of NiCo NPs; while tetralin was adsorbed and activated at NiCo sites, reacting with H* to produce decalin. The present work proposed a novel strategy to design highly efficient and stable multimetallic catalysts for heterogeneous catalytic hydrogenation reactions.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
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2025
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IF 13.1
Zilin Wang,Dongbo Shu,Haijie Chen,Chuanmin Ding,Junwen Wang,Yan Lv,Qingqing Gu,Aiqin Wang,Bing Yang
The regulation of selectivity in CO2 hydrogenation is of great importance and has been intensively studied for the utilization of CO2. The particle size and metal–support interaction are proven to be key factors influencing the selectivity of CO2 hydrogenation. However, the dynamic structure evolution during real reaction conditions and their impact on the selectivity are still poorly understood. Here in this work, we reported the crystal-phase-mediated dynamic restructuring of the Rh/TiO2 catalyst during reaction that strongly modulates the mutual interaction of dynamic size stability and strong metal–support interaction (SMSI) encapsulation of the Rh catalyst and thus the selectivity of CO2 hydrogenation toward CO/CH4. By utilizing state-of-the-art characterizations, the interplay between dynamic size distribution and SMSI of the Rh catalyst on TiO2 was clearly elucidated. The selectivity of CO2 hydrogenation was prone to the particle size in the low reaction temperature range (225–275 °C) while highly depending on SMSI at high reaction temperatures (350–400 °C). Remarkably, anatase TiO2 promotes small Rh particles and strong SMSI at the low-temperature range, rutile TiO2 facilitates large particles but high-temperature SMSI encapsulation, while the P25 phase favors large Rh particles without encapsulation. The in situ DRIFTS experiments further reveal that all Rh/TiO2 catalysts follow the hydrogenation path via *HCOO as an intermediate, where the large Rh particle size facilitates deep hydrogenation of *HCOO to CH4, whereas the TiOx encapsulation favors the *HCOO decomposition to CO due to the suppressed H2 activation. Our results provide dynamic insight for the restructuring of the active sites in the Rh/TiO2 catalyst that tunes the selectivity of CO2 hydrogenation and opens up a route for the rational design of supported metal catalysts based on their dynamic structures.
研究领域:
催化化学
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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
危险品化学品经营许可证（带存储）