Frontiers in Chemistry
·
2023
·
IF 5.5
Zhang Jie,Ren Quan,Wang Yun,Xiao Ruixue,Chen Hongyu,Xu Wenjia,Feng Yuhua
Hybrid nanostructures have garnered considerable interest because of their fascinating properties owing to the hybridization of materials and their structural varieties. In this study, we report the synthesis of [Au@Rh(OH)3]-Au island heterostructures using a seed-mediated sequential growth method. Through the thiol ligand-mediated interfacial energy, Au@Rh(OH)3 core-shell structures with varying shell thicknesses were successfully obtained. On these Au@Rh(OH)3 core-shell seeds, by modulating the diffusion of HAuCl4 in the porous Rh(OH)3 shell, site-specific growth of Au islands on the inner Au core or on the surface of the outer Rh(OH)3 shell was successfully achieved. Consequently, two types of distinct structures, the Au island-on-[Au@Rh(OH)3] dimer and Au island-Au bridge-[Au@Rh(OH)3] dumbbell structures with thin necks were obtained. Further modulations of the growth kinetics led to the formation of Au plate-Au bridge-[Au@Rh(OH)3] heterostructures with larger structural anisotropy. The flexible structural variations were demonstrated to be an effective means of modulating the plasmonic properties; the Au–Au heterostructures exhibited tunable localized surface plasmon resonance in the visible-near-infrared spectral region and can be used as surface-enhanced Raman scattering (SERS) substrates capable of emitting strong SERS signals. This diffusion-controlled growth of Au bridges in the Rh(OH)3 shells (penetrating growth) is an interesting new approach for structural control, which enriches the tool box for colloidal nanosynthesis. This advancement in structural control is expected to create new approaches for colloidal synthesis of sophisticated nanomaterials, and eventually enable their extensive applications in various fields.
研究领域:
纳米材料科学
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光学
·
化学合成
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL SCIENCES
·
2024
·Vol. 136
·期 1
·1-9
·
IF 1.7
Zhang Mingyu,Yan Dong,Xu Rui,Tang Yuqi,Xu Shuangping,Qu Yanqing,Xu Jingyu,Du Boyu,Jia Hongge
A new rhodium complex [Rh(cod)(TTT) 2 ] was synthesized by [Rh(cod)Cl] 2 as a precursor, and 4,4',4''-(1,3,5-triazine-2,4,6-triyl)trianiline (TTT) as a ligand. Its structure was verified by 1 H and 13 C NMR. The results indicate that the complex shows high activity in phenylacetylene polymerization. It was applied to the polymerization of phenylacetylene with a yield of 45.0% and Mw = 2.26×10 5 at ultra-low rhodium feed ratio ([Rh.]/[M.]=1/60000). Graphical abstract A new rhodium complex [Rh(cod)(TTT) 2 ] was synthesized by [Rh(cod)Cl] 2 as a precursor, and 4,4',4''-(1,3,5-triazine-2,4,6-triyl)trianiline (TTT) as a ligand. It was applied to the polymerization of phenylacetylene with a yield of 45.0% and Mw = 2.26×10 5 at ultra-low rhodium feed ratio ([Rh.]/[M.]=1/60000
研究领域:
无机化学
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有机金属化学
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高分子化学
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催化
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2014
·
IF 6.007
Fredrik Gunnarsson,Moa Z. Granlund,Mattias Englund,Jazaer Dawody,Lars J. Pettersson,Hanna Härelind
We report on a high NO x reduction activity over Ag/Al 2 O 3 catalysts, using hydrogen produced in a fuel reformer. The focus of the study is to evaluate the performance of a hydrocarbon selective catalytic reduction (HC-SCR) catalyst in real conditions. Initially, the catalytic materials for the fuel reformer (Rh/CeO 2 -ZrO 2 ) and the HC-SCR (Ag/Al 2 O 3 ) were evaluated in separate bench-scale reactor setups. These two setups were subsequently joined into an integrated bench-scale reactor setup with the aim to evaluate the influence of the reformate on the HC-SCR activity in a controlled environment. In the final phase of the study a 4 wt.% Ag/Al 2 O 3 catalyst doped with 100 ppm(w) Pt was scaled up and tested in a pilot-scale reactor setup. The pilot-scale reactor setup enabled evaluation of the HC-SCR activity in real exhaust gases generated by a single cylinder engine (genset) together with a hydrogen-rich gas supplied from a fuel reformer. Commercial biodiesel (NExBTL) was used as reducing agent for the HC-SCR as well as fuel in the fuel reformer for both the bench-scale and pilot-scale experiments. This study gives an excellent link between evaluations of the catalytic materials, controlled bench-scale experiments and applied engine experiments, proving a viable concept for lean NO x reduction together with onboard hydrogen production. A NO x conversion of above 70% was reached at temperatures below 250 °C, in bench-scale experiments when hydrogen produced in the fuel reformer is added.
研究领域:
环境科学
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催化化学
·
能源工程
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Junjie Wang,Zhihao Lu,Kun Gao,Xing Kang,Chengcheng Zhu,Furong Qiao,Haonan Chen,Zhuoyao Li,Wei Huang,Gang Lu
Photocatalytic reforming of ethanol provides an effective way to produce hydrogen energy using natural and nontoxic ethanol as raw material. Developing highly efficient catalysts is central to this field. Although traditional semiconductor/metal heterostructures (e.g., Rh/TiO2) can result in relatively high catalyst performance by promoting the separation of photoinduced hot carriers, it will still be highly promising to further improve the catalytic performance via a cost-effective and convenient method. In this study, we developed a highly efficient photocatalyst for ethanol reformation by preparing a ternary composite structure of Rh/TiO2/g-C3N4. Hydrogen is the main product, and the reaction rate could reach up to 27.5 mmol g–1 h–1, which is ∼1.41-fold higher than that of Rh/TiO2. The catalytic performance here is highly dependent on the wavelength of the light illumination. Moreover, the photocatalytic reforming of ethanol and production of hydrogen were also dependent on the Rh loading and g-C3N4:TiO2 ratio in Rh/TiO2/g-C3N4 composites as well as the ethanol content in the reaction system. The mechanism of the enhanced hydrogen production in Rh/TiO2/g-C3N4 is determined as the improvement in the separation of photoinduced hot carriers. This work provides an effective photocatalyst for ethanol reforming, largely expanding its application in the field of renewable energy and interface science.
研究领域:
可再生能源
·
界面科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Jingjing Zhang,Yang Feng,Lixia Ling,Caiping Ma,Jungang Wang,Riguang Zhang,Maohong Fan,Bo Hou,Debao Li,Baojun Wang
The direct conversion of syngas to ethanol faces challenges due to catalyst inefficiencies and low ethanol yield. Bulk alloys with an appropriate atomic ratio can exhibit excellent catalytic performance. In this work, a series of Rh x Ni y (111) with different Rh/Ni ratios was rationally designed, and the ethanol preparation from syngas was explored based on density functional theory (DFT) calculation and microkinetic analysis. The results show that Rh 1 Ni 1 (111) was screened out to show optimum catalytic performance for ethanol production. This was attributed to a moderate quantity of charge transfer from Ni to Rh atoms, and a medium distance from the d -band center to the Fermi level. Further, to verify the catalytic performance of the catalysts at a Rh: Ni ratio of 1: 1, 1Rh1Ni/γ-Al 2 O 3 catalyst was prepared and its catalytic performance for ethanol preparation from syngas was investigated by comparing it with that of Rh/γ-Al 2 O 3 and Ni/γ-Al 2 O 3 . The catalytic performance of 1Rh1Ni/γ-Al 2 O 3 has been further confirmed to be preferred over Rh/γ-Al 2 O 3 and Ni/γ-Al 2 O 3 , achieving a 23.0 % CO conversion rate with 31.2 % ethanol selectivity.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Qiangqiang Xue,Huilin Yi,Zhengwen Li,Zhao Jiang,Meng Chen,Yujun Wang,Binhang Yan,Guangsheng Luo
Surface modification of 600-µm-sized monodisperse gamma-alumina microspheres into magnesium–aluminum spinel, and co-impregnation-based loading of Rh–Ni (0.46 wt% Rh, 9.03 wt% Ni) were performed to synthesize catalysts for diesel-steam-reforming to hydrogen. The intimate interactions between Rh and Ni, the formation of the Rh–Ni alloy, and the Rh-doping-induced decrease in the particle size of Ni were determined. The DFT calculations results revealed that Rh-doped Ni(1 1 1) established remarkably weak bonds with oxygen-containing intermediates, and the reaction barrier of the rate-limiting step (CH 2 * + O* → CH 2 O*) on Rh–Ni(1 1 1) (0.76 eV) was lower than those of Ni(1 1 1) (1.14 eV) and Rh(1 1 1) (1.56 eV). The bimetallic catalyst shows the enhanced activity and resistance of sintering and carbon deposition compared with those of Ni-based (9.33 wt% Ni) and Rh-based (0.47 wt% Rh) catalysts. The catalytic performance of Rh–Ni-based catalyst was superior to that of physically mixed Ni-based and Rh-based catalysts at similar active metal loadings, which further confirmed the synergistic effect of Rh–Ni.
研究领域:
催化化学
·
能源材料科学
✓ 已验证
产品关联
DOI
高影响因子
Frontiers in Chemistry
·
2018
·
IF 4.155
Rao Wenxiu,Lv Guocheng,Wang Danyu,Liao Libing
Nanoscale zero valent iron has been a widespread concern in various fields due to its large specific surface area and high reactivity. However, nanoscale zero valent iron (nZVI) is very likely to aggregate and be oxidized, which limit its wide application in industry. Most clay minerals have a large adsorption capacity of cations due to their negative charges and high specific surface areas. In the present work, nZVI was loaded onto two typical clay minerals: kaolinite and sepiolite, to inhibit its oxidation and aggregation. The composites were applied to degrade Rhodamine 6G (Rh 6G) under microwave irradiation. The effects of pH value and microwave power on degradation were studied. The results showed that the removal amount of Rh 6G by nZVI/kaolinite was 110 mg/g in 15 min, while it reached 300 mg/g by nZVI/sepiolite. The difference between these two composites was mostly determined by the structures of these two clay minerals.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
Journal of Energy Chemistry
·
2023
·
IF 13.1
Qiqi Mao,Wenxin Wang,Kai Deng,Hongjie Yu,Ziqiang Wang,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
Utilizing the hydrazine-assisted water electrolysis for energy-efficient hydrogen production shows a promising application, which relies on the development and design of efficient bifunctional electrocatalysts . Herein, we reported a low-content Pt-doped Rh metallene (Pt-Rhene) for hydrazine-assisted water electrolysis towards energy-saving hydrogen (H 2 ) production, where the ultrathin metallene is constructed to provide enough favorable active sites for catalysis and improve atom utilization. Additionally, the synergistic effect between Rh and Pt can optimize the electronic structure of Rh for improving the intrinsic activity. Therefore, the required overpotential of Pt-Rhene is only 37 mV to reach a current density of −10 mA cm −2 in the hydrogen evolution reaction (HER), and the Pt-Rhene exhibits a required overpotential of only 11 mV to reach a current density of 10 mA cm −2 in the hydrazine oxidation reaction (HzOR). With the constructed HER-HzOR two-electrode system, the Pt-Rhene electrodes exhibit an extremely low voltage (0.06/0.19/0.28 V) to achieve current densities of 10/50/100 mA cm −2 for energy-saving H 2 production, which greatly reduces the electrolysis energy consumption. Moreover, DFT calculations further demonstrate that the introduction of Pt modulates the electronic structure of Rh and optimizes the d -band center, thus enhancing the adsorption and desorption of reactant/intermediates in the electrocatalytic reaction.
研究领域:
材料科学
·
电催化
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yuhua Xie,Yumei Feng,Chen Li,Fang Luo,Qing Li,Shiao Zhu,Mingxing Gong,Zehui Yang
The industrial development of acidic water splitting significantly counts on the activity associated with stability of oxygen evolution reaction (OER) electrocatalyst. In this work, we have constructed cubic Rh@Ir core–shell for acidic water splitting. The formed Rh@Ir electrocatalyst shows a high HER performance with only 29 mV overpotential for 10 mA cm −2 , stemming from the upshifted and downshifted d band center of Ir and Rh, leading to a moderate hydrogen binding strength. The Ir atom donates its electrons to nearby Rh atoms triggering a high susceptibility in nucleophilic attack by H 2 O to generate *OOH; thereby, the overpotential required to achieve 10 mA cm −2 is 216 mV for Rh@Ir core–shell, better than commercial IrO 2 . Moreover, the stability is superior to commercial IrO 2 and pure Ir electrocatalyst due to the strong electronic interplay in Rh@Ir contributing to a better resistance towards electrochemical dissolution proved by operando Raman and electrochemical impedance spectroscopies. Only 1.55 V is needed for Rh@Ir to drive overall water splitting at 10 mA cm −2 .
研究领域:
电化学
·
材料科学
·
催化
·
能源材料
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2022
·Vol. 18
·期 45
·2204490
·
IF 15.153
Bing Han,Qinghe Li,Xunzhu Jiang,Yalin Guo,Qike Jiang,Yang Su,Lin Li,Botao Qiao
The switch of CO 2 hydrogenation selectivity from CH 4 to CO over TiO 2 supported Rh catalysts is accomplished via selective encapsulation of Rh nanoparticles while exposing Rh single atoms by high-temperature reduction (HTR) according to their different strong metal-support interaction (SMSI) occurrence conditions, which can be reversed by subsequent oxidation treatment.
研究领域:
催化化学
·
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Kai Deng,Qiqi Mao,Wenxin Wang,Peng Wang,Ziqiang Wang,You Xu,Xiaonian Li,Hongjing Wang,Liang Wang
Seawater splitting is considered as a promising way to replace water splitting for H 2 production due to the enrichment of seawater resources. However, the development of this technology has been greatly hampered by the lack of efficient electrocatalysts and the detrimental effects of chlorine electrochemistry. Herein, we report a defect-rich low-crystalline Rh metallene ( l -Rh metallene) with an amorphous/crystalline hetero-phase structure for seawater electrolysis, where chlorine generation is avoided by replacing the oxygen evolution reaction (OER) with the hydrazine oxidation reaction (HzOR). Benefiting from the large surface-to-volume ratio, abundant active sites and unique electronic structure, the l -Rh metallene exhibits out-standing catalytic activity for both hydrogen evolution reaction (HER, −38 mV at 10 mA cm −2 ) and HzOR (−2 mV at 10 mA cm −2 ). Notably, an ultra-low voltage of only 28 mV is required to achieve 10 mA cm −2 in two-electrode hydrazine-assisted seawater splitting system.
研究领域:
材料科学
·
电化学
·
可再生能源
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
·
2019
·
IF 0
Caiyun Xu,Qi Li,Qiuyang Zhang,Kaijie Li,Hongfeng Yin,Shenghu Zhou
This work illustrates direct evidence of the formation of close-contact Rh-SnO2 heteroaggregate interfaces, and their enhanced catalytic hydrogenation performance is also demonstrated. Alumina-supported Rh-SnO2 heteroaggregate nanocatalysts were prepared by in situ transformation of Rh@Sn core–shell nanostructures. Various characterization techniques, especially the studies of high angle annular dark field scanning transition electron microscopy with phase mappings, confirm that Rh-SnO2 close-contact heteroaggragate nanostructures were obtained by in situ calcination and following reduction of Rh@Sn core–shell nanoparticle precursors. The catalytic studies for hydrogenations of various substituted nitroaromatics show that the Rh-SnO2/Al2O3 heteroaggregate nanocatalysts not only improve the catalytic conversions but also enhance the catalytic selectivity. The combination of characterization and catalytic studies suggests that a synergistic effect originated from close-contact Rh-SnO2 heteroaggregate interfaces exists in the Rh-SnO2 system, which enhances their catalytic hydrogenation performance.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
危险品化学品经营许可证（带存储）