MATERIALS RESEARCH BULLETIN
·
2024
·
IF 5.3
Huiyi Fang,Jin Xu,Tangyin Cui,Li Bai,Jiawei Meng,Chuncheng Wei,Xin Geng,Xiaowei Li,Haibin Sun,Guangwu Wen,Peng Wang
Ag-Rh nanocages are synthesised by a facile method at 190 °C using Ag nanocubes and Na 3 RhCl 6 as sacrificial templates and precursor, respectively. Upon introduction of Na 3 RhCl 6 into Ag nanocube suspension in ethylene glycol (EG) with poly(vinylpyrrolidone), Rh(III) ions are reduced by EG and Ag atoms via galvanic reaction; simultaneously, the released Ag(I) ions are reduced by EG. The reduction and co-deposition of both Ag and Rh atoms result in the formation of highly porous Ag-Rh nanocages when high volume of Na 3 RhCl 6 is introduced. The Ag-Rh nanocages with Ag:Rh atomic ratio of 54.2:45.8 exhibit good catalytic activity toward the degradation of rhodamine 6G, reduction of 4-nitrophenol, and decomposition of hydrazine.
研究领域:
材料科学
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催化
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纳米技术
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产品关联
DOI
高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Qiao Yuan,Yating Gu,Siquan Feng,Xiangen Song,Jiali Mu,Bin Li,Xingju Li,Yutong Cai,Miao Jiang,Li Yan,Jingwei Li,Zheng Jiang,Yingxu Wei,Yunjie Ding
Sulfur poisoning is a severe problem in industrial applications, attracting broad interest in fundamental research studies. Although a number of studies about sulfur resistance have been implemented in many reactions on nanoparticle catalysts, few investigations focus on carbonylation reactions using heterogeneous single-metal-site catalysts (HSMSCs). Herein, we present an unanticipated sulfur-promoted performance in olefin hydrocarboxylation reactions on a single-Rh-site catalyst supported on porous ionic polymers (Rh1/PIPs) with 1000 ppm H2S in CO feed. Ex situ EXAFS and in situ DRIFTS revealed a ternary cycle mechanism of olefin hydrocarboxylation reactions with Rh–H complexes as predominant active species in both pure and H2S-containing feedstock. Moreover, the transformation of the Rh mononuclear complex with the addition of H2S was also demonstrated. Density functional theory studies were performed to verify the feasibility of the proposed pathway and confirm that the energy barriers of transition states with the sulfur ligand were much lower than those in normal feed, for example, a decline of 3.4 kcal/mol for the rate-determining step of migration and insertion of CO. This work provides a distinctive example for the insight of sulfur effect on carbonylation, which could be potentially beneficial for further applications of HSMSCs.
研究领域:
催化化学
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表面科学
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理论化学
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产品关联
DOI
高影响因子
ENERGY & FUELS
·
2023
·
IF 5.3
Huizhen Dai,Te Zhang,Kaiyu Dong,Houkang Pu,Yingying Wang,Yujia Deng
Noble metal catalysts play an important role in developing efficient fuel cells for commercial application at a large scale. Among them, Pt-group metal nanocatalysts enclosed with high-index facets have been expected to exhibit high electrocatalytic activity due to the high density of the low-coordination step and kink atoms exposed on the surface. Many good studies on Pt and Pd nanocatalysts enclosed with high-index facets have been reported while Rh nanocatalysts with a high-index facet have rarely been prepared. In this work, Rh nanorods with high-index facets (310) were synthesized successfully through repeated oxygenated species adsorption/desorption mediated by square wave potential (SWP). Electrochemical tests showed that Rh nanorods with high-index facets exhibited excellent electrocatalytic activity for the formic acid oxidation reaction (FAOR), and the peak current densities in positive scan of Rh nanorods (4.48 mA·cm–2) was 4.7 times higher than that of Rh black catalysts (0.95 mA·cm–2). In addition, the Rh nanorods could maintain higher current density than that of the Rh black catalysts throughout the time domain with potential held at 0.45 V, indicating that Rh nanorods had good stability for FAOR. The enhanced electrocatalytic performance of the Rh nanorods could be mainly ascribed to high-index facets with step and kink atoms, which could provide sufficient active sites for FAOR.
研究领域:
材料科学
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电化学
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能源技术
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Qiangli Lv,Haoran Guo,Duo Xu,Yuling Zhai,Hua Wang,Tao Zhu,Xing Zhu,Kongzhai Li,Zhihong Yang,Zhishan Li
The urea oxidation reaction (UOR) is considered as an alternative to the oxygen evolution reaction for high-efficiency hydrogen production, because it can simultaneously achieve wastewater treatment and hydrogen production. However, the slow kinetics of the UOR hinder its widespread adoption due to relatively complex molecule, it is urgent to rational design and preparation of high-performance UOR catalysts. Herein, we report a simple synthesis of the NiMn-LDH@Rh(OH) 3 heterostructure and a systematic investigation of urea-assisted electrolytic hydrogen production， significantly enhances the efficiency of urea electrolysis. The amorphous Rh(OH) 3 structure provides a higher density of active sites and greater catalytic surface exposure, while the synergistic interaction between Rh(OH) 3 and NiMn-LDH improves both electrical conductivity and catalytic performance. The catalyst of NiMn-LDH@Rh(OH) 3 –3 requires only 1.29 V overpotential to achieve a current density of 10 mA cm −2 in a 1.0 M KOH and 0.33 M urea solution, surpassing other catalysts. Furthermore, it demonstrates remarkable stability with minimal potential increase during 48-hour chronopotentiometric tests at 100 mA cm −2 . This work making the developed strategy promising for the rational design of highly active electrocatalysts for green hydrogen production and the treatment of urea-rich wastewater.
研究领域:
材料科学
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能源化学
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环境科学
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产品关联
DOI
高影响因子
Molecular Catalysis
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2024
·
IF 3.9
Yifei Chen,Xinnan Zhao,Chen Xin,Xiuqin Dong,Hao Gong
This work explored the role of defective sites on the hydroformylation of n-butene through ligand regulation. The investigation examined the effect of modulator properties on defect sites and rhodium loading, and optimized the H 2 BDC/modulator ratio to improve catalyst activity. Atomically dispersed Rh is anchored to these highly dispersed defect sites, effectively preventing aggregation and thereby enhancing hydrogenation ability. Under optimal conditions, the catalyst achieved a conversion of 96.9 %, with an overall aldehyde selectivity of 90 %. DRIFTS analysis provided compelling evidence that Rh(CO) 2 and HRhCO species were formed on 1Rh/MOF-5-HBC, improving CO insertion capability. This study highlights the significance of MOFs as catalyst supports in enhancing performance through defect engineering. The ability of the modulator to induce defect formation was measured by p K a. Meanwhile, it has been discovered that the length differences between the modulator and the MOF organic ligand can have a significant impact on the stability of defective MOFs.
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 Catalysis
·
2025
·
IF 13.1
Yang Chen,Diwen Zhou,Yongli Chang,Yunzhao Xu,Hongqiao Lin,Lizhi Wu,Yu Tang,Chengyi Dai,Xingang Li,Lisheng Guo,Ting Qiu,Li Tan
The utilization of Rh-based catalysts in the direct production of ethanol from CO2 has been a subject of significant interest. However, to date, the precise active sites responsible for ethanol generation and the C–C coupling mechanism remain elusive. In this study, we present a Rh-based catalyst featuring nanoscale Rh–Fe alloy sites, which achieved an ethanol selectivity of 49.1% among all hydrocarbon and oxygenate products (CO excluded) under relatively mild reaction conditions (3.0 MPa, 200 °C, with a low metal loading of ≤1 wt %). The formation of ethanol proceeds via the HCOO* pathway with a CO insertion mechanism occurring at the alloy sites with a specific cluster size, where CH2* and CO* act as the crucial intermediates for C–C coupling. The electron interaction within the Rh–Fe alloy sites effectively reduces the energy barrier for the formation of the CH2CO* intermediate, thereby facilitating the production of ethanol. In contrast to the Rh–Fe alloy sites, the geminal-dicarbonyl binding configuration of CO* intermediates on Rh single sites favors the generation of byproducts such as methane and methanol, rather than ethanol. This research offers insights into the active sites and reaction mechanism of hydrogenation of CO2 to ethanol, thus enhancing the efficient utilization of Rh-based catalysts.
研究领域:
催化化学
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材料科学
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能源化学
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产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2023
·
IF 5.9
Xin Ning,Heming Wang,Ganghua Zhou,Longyun Zhang,Yanju Yang,Jingya Sun,Xiaozhi Wang
Ni catalysts decorated with trace Rh supported on γ-Al2O3 were prepared by the co-impregnation method. To obtain the Ni–Rh nanoparticles with different nanostructures and chemical compositions, bimetallic catalysts with varied Ni/Rh molar ratios were prepared. For comparison, monometallic Ni/γ-Al2O3 and Rh/γ-Al2O3 catalysts were also prepared by the impregnation method. The selective gas phase catalytic hydrodechlorination of 1,2-dichloroethane to ethylene was used to evaluate catalytic performances of the catalysts. The catalysts were characterized by X-ray diffraction, N2 adsorption, X-ray photoelectron spectroscopy, H2 temperature-programmed reduction, transmission electron microscopy–energy-dispersive X-ray, and CO chemisorption. It was found that the introduction of Rh to Ni catalyst facilitated the generation of spillover hydrogen which could enhance the ability of the Ni catalyst for H2 activation. In bimetallic catalysts, there was an intimate interaction between Ni and Rh, and isolated Rh sites were formed due to the dilution effect of Ni. Accordingly, compared with the monometallic Ni catalyst for gas phase catalytic hydrodechlorination of 1,2-dichloroethane, the bimetallic Ni–Rh(800)/γ-Al2O3 catalyst exhibited markedly higher 1,2-dichloroethane conversion (37%) and comparable selectivity to ethylene (95%). The findings in this study indicate that Ni–Rh/γ-Al2O3 with trace Rh can be used as a promising catalyst for highly effective and selective catalytic hydrodechlorination of chlorinated hydrocarbons.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
Journal of Physical Chemistry C
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2019
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IF 4.309
Xiu-Rong Liu,Ruo-nan Ma,Dan Zhao,Chao Chen,Ning Zhang
Deliberately modulating the surface structure of oxide semiconductor materials was crucial to improve their photoelectronic conversion performance. Here, surface engineering of a Cu2O-based semiconductor (cubic particles in an average size of 300 nm) by redox embedding Rh with RhCl63– was attempted to get a series of Rh–Cu2O catalysts, and their photocatalytic properties were typically surveyed from dye (methyl orange, MO) photodegradation. With comprehensive characterizations, it was demonstrated that the highly dispersed and tightly integrated Rh–Cu2O interface, featuring oxidatively bonded Rh in surface layers of the Cu2O substrate, was well constructed by adjusting Rh loading from 0.04 to 0.38 wt %, exhibiting an obvious enhancement in photocatalytic performance for MO degradation compared to bare Cu2O. The measurements from photoproduction of H2, photocurrent, electrochemical impedance, and scavengers-present tests further illuminated that the Rh species bonded on the Cu2O surface in an electron-deficiency state and greatly contributed to not only improving separation efficiency of photogenerated electron/hole pairs, but also lowering the resistance to speed charge transferring along the Rh–Cu2O interface, resulting in the enhanced photocatalytic performance of Rh–Cu2O catalysts. In addition, the photocatalytic principle of Rh–Cu2O catalysts for dye degradation was also discussed. These results indicated that oxidatively bonded metal species in surface layers of Cu2O was feasible for getting an efficient charge-separation–transferring M–Cu2O interface to improve the photoelectronic conversion performance, which could be referred to as a notable system to directly engineer a semiconductor surface for advanced photoenergy applications.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
ACS Applied Nano Materials
·
2025
·
IF 5.5
Wenjing Tian,Hui-Zi Huang,Di Liu,Zhejiaji Zhu,Junwen Zhou,An-Xiang Yin
The overall hydrazine splitting (OHzS, N2H4 → N2 + 2H2) reaction, which is integrated by electrocatalytic hydrazine oxidation reaction (HzOR) and hydrogen evolution reaction (HER), provides an energy-efficient alternative to conventional overall water splitting (OWS) for sustainable hydrogen production. Herein, we present the controlled synthesis of Rh1Sb1@Rh–Sb nanoflowers (NFs) that comprise intermetallic Rh1Sb1 nanodendrite cores and ultrathin Rh–Sb random alloy nanosheet shells. The alloying of Sb enhances both HzOR and HER performances of Rh nanocatalysts through modulation of growth mechanisms, morphological evolution, and surface electronic configurations. Remarkably, a symmetrical OHzS electrolyzer employing Rh1Sb1@Rh–Sb NFs as bifunctional catalysts for both electrodes achieves the current densities of 100 and 500 mA cm–2 at cell voltages of merely 0.216 and 0.700 V (without iR compensation), respectively, corresponding to 88.1% and 71.9% reductions in electricity consumption compared to alkaline OWS systems. Furthermore, a rechargeable zinc–hydrazine (Zn–Hz) battery using Rh1Sb1@Rh–Sb NFs as the positive electrode exhibits high energy efficiency, power density, and durability. The prototype device, integrating a photovoltaic cell, a Zn–Hz battery, and an OHzS cell, demonstrates the potential for efficient and simultaneous solar energy storage, hydrazine pollutant remediation, and hydrogen generation, offering a promising avenue for practical applications.
研究领域:
材料科学
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电化学
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可再生能源
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Huixian Zhong,Jiaming Wang,Shaoxia Guo,Kegong Fang,Yuan Liu
In this work, Rh–Co/La2O3–SiO2 showed excellent selectivity to ethanol for direct ethanol synthesis from syngas. The best catalyst exhibited 42.8% selectivity to ethanol with CO conversion of 12.3% and in 145 h’ running maintained stable at 553 K, 3 MPa and GHSV of 3900 mL (gcat h)−1. The investigate results indicated that the interaction of cobalt denoting electron to rhodium adjusted the amounts of carbon monoxide adsorbed associatively and dissociatively, and maybe created a new active site pair of Rh0/Coδ+ for generating ethanol. Moreover, the mutually doping effect could dilute Co and Rh atoms in Rh–Co nanoparticles (NPs), which effectively suppressed the formation of C2+H and C3+OH, and thus led to the high ethanol selectivity and good anticoking property assisting with the carbon eliminating effect of La2O3. Owing to the high dispersion of Rh–Co NPs, the catalyst showed good activity and high resistance to sintering.
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
NANOTECHNOLOGY
·
2017
·Vol. 29
·期 4
·044002
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IF 3.44
Liang Huang,Chengpeng Jiao,Liqiong Wang,Zili Huang,Feng Liang,Simin Liu,Yuhua Wang,Haijun Zhang,Shaowei Zhang
ISOBAM-104 protected Rh/Ag bimetallic nanoparticles (NPs) with average diameter less than 3.0 nm were synthesized by a co-reduction method. Ultraviolet–visible spectroscopy, transmission electron microscopy (TEM), high-resolution TEM and x-ray photoelectron spectroscopy (XPS) were employed to characterize the structure, particle size, and electronic structure of the prepared bimetallic NPs. The catalytic activities of prepared bimetallic NPs for hydrogen generation from hydrolysis of a basic KBH4 solution were evaluated in detail. The results indicated that as-prepared Rh/Ag bimetallic NPs showed a higher catalytic activity than corresponding monometallic NPs. Among all the monometallic NPs and bimetallic NPs, Rh80Ag20 bimetallic NPs exhibited the highest catalytic activity with a value of 6010 mol-H2·h−1·mol-catalyst−1 at pH = 12 and 303 K. The high catalytic activities of Rh/Ag bimetallic NPs could be attributed to presence of negatively charged Rh atoms and positively charged Ag atoms, which is supported by the results of XPS and density functional theory calculation. Based on the kinetic study, the apparent activation energy for the hydrolysis reaction of the basic KBH4 solution catalyzed by Rh80Ag20 bimetallic NPs was about 47.0 ± 3.9 kJ mol−1.
研究领域:
材料科学
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催化化学
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纳米技术
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Liang Li,Yongwei Lu,Xiaowei Liu,Xinran Wang,Siyue Zhou
Petal-like ultra-evenly Rh-doped Co 2 Fe-P composite was fabricated by a solvothermal and in-situ phosphorization strategy. Through doping a small amount of Rh within the Co 2 Fe-P structure, the catalytic activities of the composite for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) could be highly improved, and an excellent electrochemical bifunctional catalyst could be achieved. Under acidic reaction conditions, it only required an overpotential of 76 mV for HER to achieve a current density of 10 mA·cm −2 . Meanwhile, excellent electrochemical performance could also be obtained in alkaline electrolytes . The overpotential was 48 mV for HER and 303 mV for OER at 10 mA·cm −2 in 1 M KOH, respectively. Impressively, as a bifunctional electrode, the Rh doped Co 2 Fe-P composite can release a current density of 10 mA·cm −2 at a low cell voltage of 1.54 V in 1 M KOH for overall water splitting, which could be compared with that using commercial noble metal catalysts.
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
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