ELECTROCHIMICA ACTA
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2018
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IF 5.116
Jian Du,Xilong Wang,Chao Li,Xin-Yu Liu,Lin Gu,Han-Pu Liang
Studies on highly effective electrocatalysts for producing hydrogen via electrochemical water splitting is of great significance due to the increasing demand of clean and sustainable hydrogen energy economy. In this work, hollow RhCo nanoparticles with an average diameter of 21 nm were fabricated using the galvanic replacement method in a water-ice bath. Electrochemical evaluation showed that the as-synthesized electrocatalyst exhibited better performance for hydrogen evolution reaction (HER) under acid condition, with a lower overpotential of 28.1 mV at 10 mA cm −2 and a lower Tafel slope of 24 mV dec −1 , in comparison with commercial Rh/C. The better HER performance of the as-prepared hollow Rh nanoparticles could be attributed to the larger surface area than commercial Rh nanoparticles, which could provide more active sites and therefore improve the electrocatalytic performance.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2023
·
IF 13.1
Di Liu,Zhejiaji Zhu,Jiani Li,Li-Wei Chen,Hui-Zi Huang,Xiao-Ting Jing,An-Xiang Yin
The application of direct ethanol fuel cell (DEFC) has been bottlenecked by the sluggish ethanol oxidation reaction (EOR). Efficient electrocatalysts for the C−C bond cleavage are essential to promote EOR with high efficiency and C1 selectivity. Here, we prepared Rh–Cu alloy nano-dendrites (RhCu NDs) with abundant surface steps through controlled co-reduction, which exhibited significantly enhanced activity and C1 selectivity (0.47 mA cm −2 (ECSA) , 472.4 mA mg Rh −1 , and 38.9%) than Rh NDs (0.32 mA cm −2 (ECSA) , 322.1 mA mg Rh −1 , and 21.4%) and commercially available Rh/C (0.18 mA cm −2 (ECSA) , 265.4 mA mg Rh −1 , and 14.9%). Theoretical calculations and CO-stripping experiments revealed that alloying with Cu could modulate the surface electronic structures of Rh to resist CO-poisoning while strengthening ethanol adsorption. In situ Fourier transform infrared spectroscopy (FTIR) indicated that the surface steps on RhCu NDs further promoted the C−C bond cleavage to increase the C1 selectivity. Therefore, optimizing the surface geometric and electronic structures of nanocrystals by rational composition and morphology control can provide a promising strategy for developing practical DEFC devices.
研究领域:
材料科学
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电化学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 4
·1623-1628
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IF 8.867
Binbin Jiang,Yuyang Sun,Fan Liao,Wen Shen,Haiping Lin,Hui Wang,Mingwang Shao
Hydrogen production with the aid of electrocatalysis is a critical component for several developing clean-energy technologies. Such a renewable energy depends heavily on the choice of cheap and efficient catalysts for hydrogen evolution, which has still been a challenge until now. In this work, the theoretical calculation indicates that Rh–Ag–Si ternary catalysts exhibit more active hydrogen evolution performance than Pt–Ag–Si because the migration activation energies of H atoms from Rh(111) to Si are lower than those from Pt(111) to Si via the Ag surface. This simulation was confirmed by the experimental results: Rh–Ag/SiNW (or Pt–Ag/SiNW) catalysts were prepared by directly reducing Rh (or Pt) and Ag ions with Si–H bonds. The Rh–Ag/SiNW-2 with the optimal mass ratio of 2.3 : 23.4 : 74.3 (Rh : Ag : Si) exhibited a lower Tafel slope (51 mV dec−1) and a larger exchange current density (87.1 × 10−6 A cm−2) than the Pt–Ag/SiNW. In addition, the mass activity of Rh–Ag/SiNW-2 at an overpotential of 0.2 V (11.5 mA μgRh−1) is 12.0, 5.0 and 3.3 fold higher than that of Rh–Ag (0.96 mA μgRh−1), Pt–Ag/SiNW (2.3 mA μgPt−1) and 40 wt% Pt/C (3.5 mA μgPt−1) catalysts, respectively. Moreover, the Rh–Ag/SiNW nanocatalysts had good stability in acidic media. The results presented herein may offer a novel and effective methodology for the designing of cost-efficient and environmentally friendly catalysts for electrochemical fields.
研究领域:
材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2020
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IF 7.1
Ao Liu,Siyuan Lv,Lianjing Zhao,Fangmeng Liu,Jing Wang,Rui You,Zijie Yang,Junming He,Li Jiang,Chenguang Wang,Xu Yan,Peng Sun,Geyu Lu
In this work, polyaniline (PANI) coated Rh-doped SnO 2 hollow nanotubes (PRS) were synthesized via electrostatic spinning and in-situ polymerization technique. The obtained samples were characterized by X-ray diffractometer, Field emission scanning electron microscopy, Transmission electron microscopy, X-ray photoelectron spectroscopy and Brunauer-Emmett-Teller. The gas sensing performances of the sensors based on PRS nanotubes were investigated systematically at room temperature. It was shown that the polyaniline coated 0.5 mol% Rh-doped SnO 2 nanotube (PRS0.5) sensor exhibited the highest response value of 13.6 to 100 ppm NH 3 at room temperature with excellent selectivity, acceptable repeatability and favorable flexibility. The enhanced gas sensing performances were due to the morphology structure, the heterojunction between PANI and Rh-SnO 2 and the catalytic effect of Rh 2 O 3 . Thus, the PANI coated Rh-doped SnO 2 hollow nanotubes could be a promising candidate for designing and fabricating flexible NH 3 gas sensor at room temperature.
研究领域:
材料科学
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传感器技术
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2019
·
IF 4.084
Qilu Yao,Meng He,Xiaoling Hong,Xinyu Chen,Gang Feng,Zhang-Hui Lu
Hydrazine borane (N 2 H 4 BH 3 , 15.4 wt%) and hydrous hydrazine (N 2 H 4 ·H 2 O, 8 wt%) are promising chemical hydrogen storage materials that have attracted much attention in recent years due to their high gravimetric hydrogen capacities. The selective and rapid catalytic dehydrogenation of N 2 H 4 BH 3 and N 2 H 4 ·H 2 O is the key to the potential use of the abovementioned materials in hydrogen applications. In this study, a series of Rh-MoO x nanoparticles (NPs) with various metal compositions have been successfully prepared via a simple one-step chemical reduction approach in the absence of a surfactant/support at room temperature . The obtained surfactant/support-free Rh-MoO x NPs exhibit good dispersibility and small particle size. Among all of the as-prepared Rh-MoO x NPs, the optimized Rh-MoO x catalysts with a molar ratio of 1:1 show the highest catalytic properties with 100% H 2 selectivity for hydrogen evolution from aqueous N 2 H 4 BH 3 and N 2 H 4 ·H 2 O solutions at 323 K under alkaline conditions. The turnover frequency (TOF) values of Rh 0.5 (MoO x ) 0.5 NPs are 2000 and 750 h −1 for hydrogen evolution from N 2 H 4 BH 3 and N 2 H 4 ·H 2 O , respectively, which are among the highest values ever reported for Rh-based catalysts. The superior catalytic performances could be attributed to the small particles size, low crystallinity , modified electronic structure, and strong basic sites of Rh NPs induced by the MoO x dopant . The highly rapid and selective Rh-MoO x catalyst may further encourage the deployment and application of N 2 H 4 BH 3 and N 2 H 4 ·H 2 O as safe and convenient sources of hydrogen for fuel cells.
研究领域:
化学工程
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材料科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
Environmental Science-Nano
·
2020
·Vol. 7
·期 8
·2267-2277
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IF 7.683
Qian Zhou,Qingyun Shi,Najun Li,Dongyun Chen,Qingfeng Xu,Hua Li,Jinghui He,Jianmei Lu
Coupling the piezoelectric effect of piezoelectric semiconductors with the photocatalytic technique is considered as a promising strategy for suppressing the recombination of photogenerated charge carriers. A new piezo-photocatalyst, a Rh-doped SrTiO3 inverse opal, was prepared by a hard-template method. Doping of photoactive Rh3+ played a significant role in improving the visible-light response ability and piezo-/photocatalytic activity of SrTiO3. In addition, the introduction of 3D ordered inverse opal structure was favourable for light harvesting. Co-excited by solar energy (visible light) and mechanical energy (ultrasonic vibration), the Rh-doped SrTiO3 inverse opal showed a significantly enhanced degradation rate of bisphenol A, which was 8.9 times higher than that of SrTiO3 nanoparticles under visible light only. The boosted piezo-photocatalytic efficiency was ascribed to the efficient separation of photogenerated electron–hole pairs under the acceleration of the built-in piezoelectric field in the Rh-SrTiO3 inverse opal, as confirmed by piezoelectric force microscopy (PFM). Therefore, this work provided a new insight into SrTiO3-based piezo-photocatalytic materials for efficient environmental remediation.
研究领域:
材料科学
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环境科学
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化学
✓ 已验证
DOI
高影响因子
Molecular Catalysis
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2021
·
IF 5.062
Xiao Li,Liusha Li,Tingting Qin,Gong Gun,Tiejun Lin,Liangshu Zhong
Tandem hydroaminomethylation is an efficient and green route for one-pot synthesis of amines directly from olefins. Herein, heterogeneous hydroxyapatite (HAP) supported single-atom Rh catalyst was prepared and used for tandem hydroaminomethylation of olefins. Characterization techniques confirmed the atomic dispersion of Rh species on HAP. Up to 99% conversion of 1-hexene with high selectivity to the desired amines (93.2%) was obtained over 0.5Rh 1 /HAP catalyst. Mechanism study demonstrated that the first hydroformylation step during the tandem catalytic process was rate-determining. Compared with the Rh nanoparticles on other oxide supports (Mg 3 Al, MgO and Al 2 O 3 ), the atomically dispersed Rh sites on HAP ensured the high hydroformylation activity, thereby guaranteed the outstanding catalytic performance for the total tandem process. Furthermore, various corresponding amines can be obtained with satisfactory yields over 0.5Rh 1 /HAP catalyst from a wide scope of olefins or amines substrates.
研究领域:
催化化学
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材料科学
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绿色化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Caixia Zhu,Kaizhuang Xu,Yuan Fang,Qian Lv,Kun Jiang,Huibo Zhao,Yang Chen,Peng Wang,Hua Yang,Lizhi Wu,Yu Tang,Li Tan
The direct synthesis of ethanol from syngas is a promising way in the field of clean and efficient use of fossil fuel, but it still suffers from insufficient ethanol selectivity and understanding of active sites. In this work, the Rh-based catalyst with Ce as promoter and ZrO 2 as carrier exhibits excellent catalytic performance, showing the selectivity of ethanol toward 24.3 %. Moreover, the yield of methane decreases to 4.8 %, and the formation of CO 2 is inhibited to a certain degree by tuning the active sites. The carrier is changed by doping Ce into the ZrO 2 lattice, which assists to form the Rh δ+ active sites. The synergetic effect of Ce and Zr is important to influence the state of Rh species in the catalysts, leading to the differences in the CO hydrogenation process. On the other hand, the Rh δ+ active sites are also stabilized by promoted surface oxygen vacancies in the 2.0Rh5.0Ce-ZrO 2 catalyst. The high-activity catalyst with Rh δ+ active sites will be helpful to understand the real active sites of Rh-based catalysts for ethanol synthesis from syngas, thereby guiding further design of the related catalyst with high performance to meet the industrial demand in syngas converting to ethanol.
研究领域:
催化化学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
HYDROMETALLURGY
·
2019
·
IF 3.465
Shunyan Ning,Shichang Zhang,Wei Zhang,Jie Zhou,Siyi Wang,Xinpeng Wang,Yuezhou Wei
The separation of fission products Ru, Rh, and Pd will benefit both the nuclear fuel cycle and enlarge the platinum group metals source. A silica-based iso Bu-BTP/SiO 2 -P adsorbent was used to separate Ru, Rh, and Pd from nitrate solution. It exhibited good adsorption towards Ru, Rh, and Pd with the uptake rates over 95% at 55 °C in 0.1 M HNO 3 –3 M NaNO 3 solution and no adsorption towards 238 U(VI). The adsorption towards Ru, Rh, and Pd matched well with pseudo-second-order model with the equilibrium obtained within 24 h, 24 h and 0.5 h and Langmuir adsorption isotherm model with the saturation adsorption amounts as high as 0.37 mmol/g, 0.34 mmol/g and 0.71 mmol/g respectively. The adsorbed Pd, Rh, and Ru can be desorbed by 0.1 M HNO 3 –0.1 M thiourea , 2 M HCl and NaClO solution (CP) which is expected to realize their mutual separation in desorption stage using the above-mentioned eluents successively. Both FT-IR and XPS revealed that C N C played key role during adsorption and the adsorption needed the participation of NO 3 − to keep charge balance. In a word, iso Bu-BTP/SiO 2 -P is a promising adsorbent for separation and recovery Ru, Rh, and Pd, especially in the case of separating them from other fission products and actinides from high level liquid waste .
研究领域:
核化学
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材料科学
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放射化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 4
·312
·
IF 4
Yuqiao Li,Shaoyuan Sun,Dezheng Li,Huimin Liu,Yiming Lei
Photothermal catalytic dry reforming of methane (DRM) technology not only achieves artificial photosynthesis of fuels but also decreases greenhouse effects. The highly efficient photothermal DRM reaction depends on elaborate catalysts. Therefore, unraveling the relationship between property and catalytic efficiency of catalysts is crucial. In this study, a series of Rh-loaded Ga2O3-Nb2O5(Rh/GaxNby) were designed via a simple in situ reduction strategy using Rh2O3/Ga2O3-Nb2O5as a precursor. After an accurate material characterization, as a proof-of-principle, the photothermal efficiency could be attributed to (i) the amount of medium and strong basic sites on the catalyst surface; (ii) the number of electron–hole pairs upon visible light irradiation. Accordingly, this study used Rh/GaxNbyas a model hybrid catalyst to clarify the relationship between the fundamental properties and photothermal catalytic DRM activities, thus providing guidance for the rational design and fabrication of efficient metal/semiconductor composite catalysts for DRM implementation.
研究领域:
化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
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2015
·
IF 3.615
Miao Jiang,Li Yan,Yunjie Ding,Qi Sun,Jia Liu,Hejun Zhu,Ronghe Lin,Fengshou Xiao,Zheng Jiang,Jingyue Liu
The heterogenization of homogeneous catalysts is of critical importance for both fundamental research and practical applications. The key obstacle to industrial applications of heterogenized homogeneous catalysts is the long-term stability of the immobilized molecular complexes. We unambiguously demonstrate in this report that the vinyl-functionalized PPh 3 polymers supported single Rh sites (Rh/POL–PPh 3 ) catalyst provided not only excellent catalytic activity but also ultrahigh stability for fixed-bed olefins hydroformylation , which is one of the most important industrial homogeneous catalytic processes for the synthesis of aldehydes and alcohols. HAADF-STEM and EXAFS results indicated that the Rh atoms were present in single Rh sites which were strongly coordinated with the exposed phosphorous atoms of the POL–PPh 3 support. The Rh/POL-PPh 3 catalyst provided high activity and selectivity because it maintained the catalytic functionalities similar to the homogeneous HRh(CO)(PPh 3 ) 3 complex, as demonstrated both by 31 P MAS NMR and in situ FT-IR experiments. Thus a reaction mechanism, similar to that over the homogeneous HRh(CO)(PPh 3 ) 3 complex, was proposed for olefin hydroformylation over the novel Rh/POL–PPh 3 catalyst.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Junji Chen,Heshan Cai,Tianxiang Zhao
Aluminium oxide (Al 2 O 3 ) is a promising catalyst support due to its excellent stability, high specific surface area, low price, and wide applicability. At present, most of the synthesis methods of Al 2 O 3 are wet chemical process, and the solid-state synthesis of catalysts is underdeveloped under solvent-free conditions. In this study, we proposed a novel strategy for solvent-free synthesis of Rh/Al 2 O 3 catalysts via mechanochemistry. The pore properties of the catalysts can be tuned by simply adjusting the amount of template CTAB and calcination temperatures. As a proof of concept, as-prepared catalysts are used to catalyze hydrolytic dehydrogenation of ammonia borane. The best catalyst Rh/Al 2 O 3 -CTAB(0.4)-500 achieves a total turnover frequency of 186.0 mol H2 ·mol Rh −1 ·min −1 at 298 K and the activation energy is 44.8 kJ·mol −1 . It also exhibits good cycling properties for catalyzing the hydrolysis of ammonia borane completely even after five runs. The catalysts were also characterized by various methods, including SEM, TEM, XPS, XRD, etc., to study the relationship between their structure and catalytic performance. The results show that the high activity of the catalyst is closely related to its large BET specific surface area and appropriate average pore size.
研究领域:
材料科学
·
催化化学
✓ 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）