ACS Applied Energy Materials
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2021
·
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.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
·
IF 4.939
Wei Cheng,Yumei Peng,Yi Wang,Weidong Jiang,Yan Long,Guangyin Fan
Hydrogen evolution from ammonia borane (AB) hydrolysis is of great importance considering the ever-increasing demand for green and sustainable energy. However, the development of a facile and efficient strategy to construct high-performance catalysts remains a grand challenge. Herein, we report an amino-group and space-confinement assisted strategy to fabricate Rh nanoparticles (NPs) using amino-functionalized metal-organic-frameworks (UiO-66-NH 2 ) as a NP matrix (Rh/UiO-66-NH 2 ). Owing to the coordination effect of amino-group and space-confinement of UiO-66-NH 2 , small and well-distributed Rh NPs with a diameter of 3.38 nm are successfully achieved, which can be served as efficient catalysts for AB hydrolysis at room temperature . The maximum turnover frequency of 876.7 min −1 is obtained by using the Rh/UiO-66-NH 2 with an optimal Rh loading of 4.38 wt% and AB concentration of 0.2 M at 25 °C, outperforming most of the previously developed Rh-based catalysts. The catalyst is also stable in repetitive cycles for five times. The high performance of this catalyst must be ascribed to the structural properties of UiO-66-NH 2 , which enable the formation of small and well-dispersed Rh NPs with abundant accessible active sites. This study provides a simple and efficient method to significantly enhance the catalytic performance of Rh for AB hydrolysis.
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Nanoscale Advances
·
2019
·Vol. 1
·期 10
·3941-3947
·
IF 0
Xiao Li,Yucong Yan,Yi Jiang,Xingqiao Wu,Shi Li,Jingbo Huang,Junjie Li,Yangfan Lin,Deren Yang,Hui Zhang
Hydrolysis of ammonia borane (AB) is a safe and convenient means of H2 production when efficient catalysts are used. Here we report a facile one-pot solvothermal method to synthesize Rh/WO3−x hybrid nanowires. Ultra-small Rh nanoparticles with an average size of ∼1.7 nm were tightly anchored on WO3−x nanowires. Rh/WO3−x catalysts exhibited substantially enhanced activity for hydrolytic dehydrogenation of AB under both dark and visible light irradiation conditions relative to mixed Rh nanoparticles and WO3−x nanowires (Rh + WO3−x), and Rh/C and WO3−x nanowires. X-ray photoelectron spectroscopy (XPS) analysis indicated that the synergistic effect between Rh nanoparticles and WO3−x nanowires was responsible for such an enhancement in activity. Specifically, Rh/WO3−x achieved the highest turnover frequency (TOF) with a value of 805.0 molH2 molRh−1 min−1 at room temperature under visible light irradiation. The H2 release rate as a function of reaction time exhibited a volcano plot under visible light irradiation, indicating that a self-activation process occurred in the hydrolytic dehydrogenation of AB due to additional oxygen vacancies arising from in situ reduction of WO3−x nanowires by AB, and thus an enhanced localized surface plasmon resonance (LSPR). Such a self-activation process was responsible for the enhanced catalytic activity under visible light irradiation relative to that under dark conditions, which was supported by the lower activation energy (45.2 vs. 50.5 kJ mol−1). In addition, Rh/WO3−x catalysts were relatively stable with only little loss in activity after five cycles due to the tight attachment between two components.
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JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Yuqing Wang,Li Yan,Cunyao Li,Miao Jiang,Ziang Zhao,Guangjin Hou,Yunjie Ding
Porous organic copolymer (designated as CPOL-BP&P(OPh) 3 ) containing vinyl biphephos moieties and tris(4-vinylphenyl)phosphite (P(OPh) 3 ) moieties was synthesized through a solvothermal copolymerization technique. After metalation with Rh precursor, an efficient heterogeneous catalyst Rh/CPOL-BP&P(OPh) 3 for the hydroformylation of 1-butene is presented with high activity (TOF = 2490.3 h −1 ) and regioselectivity (l:b = 40.0). The Rh/CPOL-BP&P(OPh) 3 catalyst has been investigated by using solid-state 13 C MAS NMR, in situ FT-IR spectroscopy, nitrogen sorption measurements, SEM, TEM, and XPS. Interestingly, in situ FT-IR spectra showed that Rh species tended to coordinate with both two kinds of P species from biphephos and P(OPh) 3 ligands in the Rh/CPOL-BP&P(OPh) 3 polymer frame rather than one kind of them. Therefore, the synergistic effect of three kinds of coordination compound formed between Rh species and both ligands could be responsible for the high activity and regioselectivity observed in hydroformylation of 1-butene.
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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.
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RSC Advances
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2017
·Vol. 7
·期 6
·3161-3169
·
IF 3.108
Fuhai Li,Hanqin Weng,Yun Shang,Zuoming Ding,Zheng Yang,Sheng Cheng,Mingzhang Lin
Rhodium (Rh) is one of the most important catalyst constituents in many industrial catalytic processes. The synthesis of rhodium nanoparticles (RhNps) has received considerable interest for decades. In this paper, we report an environmentally friendly and facile synthesis route of RhNps through direct reduction of RhCl3 by ethanol in an alkaline medium in the presence of PVP at room temperature, confirmed by UV-vis spectroscopy, TEM, XRD and XPS. The effects of the concentrations of OH− and ethanol, as well as the nature of the alcohols, which greatly affected the formation rate of RhNps, were systematically investigated to understand the mechanism. Our results support that ethoxy anions generated from the deprotonation of ethanol were highly active and responsible for the formation of RhNps. Electrochemical tests have shown that Rh/C displayed zero activity in an acid medium, while in an alkaline medium Rh/C was highly active and displayed enhanced catalytic activity towards ethanol oxidation compared to commercial Rh/C. The process presented in this work is expected to be useful for preparing Rh-based nanocatalysts at room temperature, which may be extended to other nanocatalysts.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
·
IF 7.139
Ying Duan,Pan Guo,Dong Sui,Dongsheng Deng,Tianliang Lu,Yanliang Yang
The development of a cost-effective catalyst for hydrogen evolution from ammonia borane is of importance for the application of AB as a hydrogen storage material. In this manuscript, a series of noble metal catalysts M@CuOx/C (M = Ru, Rh, Pd, and Pt) are prepared by the galvanic reduction method. The catalysts are characterized by XRD , TEM , EDS mappings and lines scanning, XPS , HAADF-STEM, and ICP-OES. The noble metal is highly dispersed on the surface of Cu nanoparticles . The morphology of Cu nanoparticles changed according to different metals after the introduction of noble metal and there has an interaction between the noble metal and Cu. The M@CuOx/C is used for the hydrolysis of AB. For the same metal catalyst, the activity of M@CuOx/C is increased by about 3–7 times than the corresponding M/C at 298 K. The Rh shows the highest TOF and lowest activation energy among the four noble metals.
研究领域:
材料科学
·
催化化学
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Small
·
2026
·
IF 11.8
Wuxi Zhang,Jianyu Li,Yangke Cun,Xinmin Bai,Yingzhu Zi,Zan Xu,Jianbei Qiu,Zhaoyu Ma,Junying Zhang,Zhengwen Yang
Most widely-studied semiconductor catalysts have low efficiency in utilizing near-infrared (NIR) light in the solar spectrum, while also facing major issues such as slow charge-carrier migration rate and lack of active sites that limit photocatalytic performance. Here, a new strategy to promote the solar-light driven photocatalytic activity of ZnIn 2 S 4 was proposed by introducing Rh single atom (SAs) into CeO 2 :Yb,Er/ZnIn 2 S 4 with photo-thermo-electric effects. The introduction of Rh SAs into ZnIn 2 S 4 effectively suppresses charge recombination, and improves reaction rate through photo-thermal effect. CeO 2 :Yb, Er converts NIR light into visible light via up-conversion photo-optical processes and generates high-energy electrons via two-photon photo-electronic process, both of which can activate ZnIn 2 S 4 . Large contact area and strong interface electric field between CeO 2 and ZnIn 2 S 4 enhance photo-electric conversion efficiency. The CeO 2 :Yb,Er/Rh-ZnIn 2 S 4 exhibits a hydrogen production rate of up to 99.68 mmol·g −1 ·h −1 at 10°C and 148.06 mmol·g −1 ·h −1 with non-temperature-controlled conditions. Under mild conditions, the photocatalysts can convert glucose into high-value-added chemicals (e.g., arabinose) while simultaneously generating hydrogen. This work provides a new strategy to improve NIR light utilization efficiency and enhance charge-carrier separation capability through photo-thermo-electric effects, promoting the production of green hydrogen and biomass conversion into high-value-added chemicals.
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高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
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2020
·Vol. 35
·期 2
·e6104
·
IF 3.14
Kuan Wang,Jie Lan,Zhen-Hong He,Zhe Cao,Weitao Wang,Yang Yang,Zhao-Tie Liu
The synthesis of benzyl alcohols (BAs) is highly vital for their wide applications in organic synthesis and pharmaceuticals. Herein, BAs was efficiently synthesized via hydroxymethylation of phenylboronic acids (PBAs) and paraformaldehyde over a simple Rh PPh 3 catalyst combined with an inorganic base (NaOH). A variety of BAs with the groups of CH 3 − , CH 3 O − , Cl − , Br − , and so on were obtained with moderate to good yields, indicating that the protocol had a good universality. Density functional theory (DFT) calculations proposed the Hayashi-type arylation mechanism involved the arylation step of PBA and Rh(OH)(PPh 3 ) 2 catalyst to form Rh(I)-bound aryl intermediates and the hydrolysis step of Rh(I)-bound aryl intermediates and HCHO to generate BA product (the rate-determining step). The present route provides a valuable and direct method for the synthesis of BAs and expands the application range of paraformaldehyde.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2014
·
IF 4.331
Yanlin Ren,Guangyin Fan,Chenyu Wang
Reduced graphene oxide (RGO) supported rhodium nanoparticles (Rh-NPs/RGO) was synthesized through one-pot polyol co-reduction of graphene oxide (GO) and rhodium chloride. The catalytic property of Rh-NPs/RGO was investigated for the aqueous phase hydrodechlorination (HDC) of 4-chlorophenol (4-CP). A complete conversion of 4-CP into high valued products of cyclohexanone (selectivity: 23.2%) and cyclohexanol (selectivity: 76.8%) was successfully achieved at 303 K and balloon hydrogen pressure in a short reaction time of 50 min when 1.5 g/L of 4-CP was introduced. By comparing with Rh-NPs deposited on the other supports, Rh-NPs/RGO delivered the highest initial rate (111.4 mmol/g Rh min) for 4-CP HDC reaction under the identical conditions. The substantial catalytic activity of Rh-NPs/RGO can be ascribed to the small and uniform particle size of Rh (average particle size was 1.7 ± 0.14 nm) on the surface of the RGO sheets and an electron-deficient state of Rh in the catalyst as a result of the strong interaction between the active sites and the surface function groups of RGO.
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高影响因子
MICROVASCULAR RESEARCH
·
2025
·
IF 2.7
Jiang Hugang,Liu Ai,Guo Zeao,Ren Chunzhen,Lin Wenyan,Liu Kai,Zhao Xinke,Li Yingdong
Background Coronary Microvascular Dysfunction (CMVD), a prevalent comorbidity of various cardiovascular diseases, may contribute to myocardial cell ischemic necrosis. The loss of microvessels—driven by endothelial cells (ECs) apoptosis—is the core pathological hallmarks of CMVD. Our previous studies have established that RAS-RH ( Angelica sinensis and Astragalus membranaceus ultrafiltrate) promotes angiogenesis and improves cardiac perfusion. However, its underlying molecular mechanisms remain incompletely understood. Purpose This study aimed to elucidate the key mechanism by which quercetin, the primary active component of RAS-RH, modulates radiation-induced ECs apoptosis. Methods Through the integration of network pharmacology and transcriptomics, we identified potential active components of RAS-RH and their key targets involved in regulating the telocytes-endothelial cell (TCs-ECs) crosstalk pathway underlying CMVD. These predictions were further validated using in vitro cellular models via flow cytometry, western blot, wound-healing assays, in situ hybridization, immunofluorescence staining, and EdU proliferation assays. Results Consistent with our predictions, experimental results demonstrated that quercetin (the primary active component of RAS-RH) significantly upregulated the expression of HIF-1α and miRNA-126 in TCs ( P < 0.01) and enhanced miRNA-126 paracrine secretion. Through this paracrine mechanism, quercetin downregulated the expression of Cypd, ANT, F1F0-ATPase, and VDAC in ECs ( P < 0.01), inhibited the reduction of mitochondrial membrane potential (ΔΨm) and ECs apoptosis induced by excessive mPTP opening. Collectively, these effects enhanced ECs proliferation, migration, and tube formation capacity, ultimately promoting angiogenesis. Conclusion These results collectively demonstrate that quercetin, the primary active component of RAS-RH, suppresses excessive mPTP activation and apoptosis while stimulating ECs migration and tube formation. This occurs via upregulating HIF-1α and miRNA-126 expression in TCs and enhancing miRNA-126 paracrine to ECs, positioning the TCs-ECs crosstalk mechanism as a promising novel therapeutic target for intervening in coronary microcirculation dysfunction.
研究领域:
心血管药理学
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分子生物学
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辐射生物学
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网络药理学
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转录组学
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血管生成研究
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高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Ke Jia,Yawei Wang,Lixia Jiang,Mi Lai,Wenlan Liu,Liping Wang,Huihui Liu,Xiaohua Cao,Yuze Li,Zongxiu Nie
Lung cancer ranks among the cancers with the highest global incidence rates and mortality. Swift and extensive screening is crucial for the early-stage diagnosis of lung cancer. Laser desorption/ionization mass spectrometry (LDI-MS) possesses clear advantages over traditional analytical methods for large-scale analysis due to its unique features, such as simple sample processing, rapid speed, and high-throughput performance. As n-type semiconductors, titanate-based perovskite materials can generate charge carriers under ultraviolet light irradiation, providing the capability for use as an LDI-MS substrate. In this study, we employ Rh-doped SrTiO3 (STO/Rh)-assisted LDI-MS combined with machine learning to establish a method for urine-based lung cancer screening. We directly analyzed urine metabolites from lung cancer patients (LCs), pneumonia patients (PNs), and healthy controls (HCs) without employing any pretreatment. Through the integration of machine learning, LCs are successfully distinguished from HCs and PNs, achieving impressive area under the curve (AUC) values of 0.940 for LCs vs HCs and 0.864 for LCs vs PNs. Furthermore, we identified 10 metabolites with significantly altered levels in LCs, leading to the discovery of related pathways through metabolic enrichment analysis. These results suggest the potential of this method for rapidly distinguishing LCs in clinical applications and promoting precision medicine.
研究领域:
癌症研究
·
质谱分析
·
机器学习
·
代谢组学
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高影响因子
危险品化学品经营许可证（带存储）