INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Hongyu Niu,Yuan Cheng,Chuang Li,Shaojie Li,Jingjie Luo,Changhai Liang
Rational design of promising Cu catalyst requires better understanding of the Cu–support perimeter for reactions such as hydrogenation rearrangement of furfural─a pivotal and alternative transformation to produce cyclopentanol. Herein, a series of Cu catalysts with constructed Cu-M-Ox interfaces (M = Zn or Al) have been synthesized. In freshly reduced Cu/ZnO-Alx samples, aluminum species was enriched surrounding Cu. The Cu-Al-Ox contacting interface was formed, and the CuAl2O4 spinal structure was detected as a combining consequence only if Zn and Al species coexisted. The specific metal–support synergistic interaction and Cu-Al-Ox contacting interface simultaneously aroused the enhanced redox property and large number of surface acid sites, facilitating the adsorption/activation of hydrogen and reactants. During the reaction, Al2O3 retreating from the Cu-Al-Ox interface caused the replacement of Cu-Al-Ox by new Cu-Zn-Ox interface, which was directly correlated with the irreversibly changed chemical structure and decreased cyclopentanol yield, although the furfural conversion was well sustained. In this work, we confirmed that supported copper catalysts were competent for the activation and conversion of furfural, with the turnover frequency reaching 28.1 h–1 by the Cu/ZnO-Al3 sample at temperatures as low as 90 °C. The further transformation of cyclopentanone to cyclopentanol was largely depending on the maintenance of a steady Cu-Al-Ox contacting interface.
研究领域:
催化
·
化学工程
·
材料科学
·
有机化学
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Jiancai Hou,Jiangliang Hu,Liping Chang,Jiancheng Wang,Zequan Zeng,Dongxia Wu,Xinmin Cui,Weiren Bao,Junxuan Yao
Cu-Ce mixed oxides with different Cu contents were synthesized through a sol–gel method, after which their effect on benzene combustion catalysis was evaluated. CeCu0.50 calcined at 300 °C (CeCu0.50–300) exhibited a high areal rate [2.0 × 10 −6 mol/(m 2 h)] and turnover frequency (0.16 s −1 ) at 170 °C, thus demonstrating the strong synergistic effect between CuO and CeO 2 . The catalyst durability and influence of H 2 O(g) on catalytic activity were also investigated. Correlation analyses between the catalytic activities and the amount of copper species, indicated that CuO x clusters and the Cu-[O x ]-Ce structure were the main active sites and bridge for oxygen transfer, respectively. Furthermore, benzene did not adsorb onto the copper species. The effect of temperatures on surface oxygen vacancies and oxygenated intermediates were also evaluated. Taken together, our findings provided key insights into the synergistic effects of different copper species on benzene combustion.
研究领域:
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Houlin Wang,Shuting Luo,Meisheng Zhang,Wei Liu,Xiaodong Wu,Shuang Liu
Though the catalytic oxidation of CO, NO and soot over CeO 2 could be understood within a similar Mars-van Krevelen-type mechanism, these reactions were likely to be driven by different active phases. In this work, several CeO 2 and Ag/CeO 2 nanorods with different contents of surface oxygen vacancies (V O-s ) and active oxygen species (O x − ) were designed as model catalysts. Their catalytic performance indicated that, CO oxidation was determined by pre-existing ceria V O-s , while O x − participated in NO and soot oxidation directly. Besides, by loading silver onto the high-temperature aged CeO 2 nanorods, Ag/CeO 2 catalysts with high availability of ceria lattice oxygen were obtained, whose low-temperature oxidation activity was proven comparable to that of the platinum catalysts. In this sense, the model designing in this work not only provided methods to find out proper reactivity descriptors, but also conferred low-cost catalysts with high practical potential.
研究领域:
催化
·
材料科学
·
化学工程
·
环境化学
✓ 已验证
DOI
高影响因子
Small
·
2022
·Vol. 18
·期 23
·2201200
·
IF 15.153
Peng Jing,Peixin Liu,Minghao Hu,Xuan Xu,Baocang Liu,Jun Zhang
Electrochemical nitrogen reduction powered by renewable electricity is a promising strategy to produce ammonia. However, the lack of efficient yet cheap electrocatalysts remains the biggest challenge. Herein, hybrid Cu 2 O-CeO 2 -C nanorods are prepared on copper mesh through a metal-organic framework template route. The Cu-loaded Ce-MOF is thermally converted to Cu 2 O-CeO 2 heterojunctions with interfacial Cu-[O X ]-Ce structures embedded in carbon. Theoretical calculations reveal the lower formation energy of oxygen vacancies in Cu-[O X ]-Ce structures than in the Cu 2 O or CeO 2 phase. The Cu-[O X ]-Ce structures with oxygen vacancies enable the formation of interfacial electron-rich Cu(I) species which show significantly enhanced performance toward electrocatalytic nitrogen reduction with an NH 3 yield of 6.37 × 10 −3 µg s −1 cm −2 and a Faradaic efficiency of 18.21% in 0.10 m KOH at −0.3 V versus reversible hydrogen electrode. This work highlights the importance of modulation of charge distribution of Cu-based electrocatalysts to boost the activity toward nitrogen reduction.
研究领域:
电化学
·
材料科学
·
催化
·
可再生能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Zhang Yue,Mu Xueqin,Liu Zhengyang,Zhao Hongyu,Zhuang Zechao,Zhang Yifan,Mu Shichun,Liu Suli,Wang Dingsheng,Dai Zhuhui
The development of efficient and robust catalysts for hydrogen evolution reaction is crucial for advancing the hydrogen economy. In this study, we demonstrate that ultra-low coordinated hollow PtRuNi-O x nanocages exhibit superior catalytic activity and stability across varied conditions, notably surpassing commercial Pt/C catalysts. Notably, the PtRuNi-O x catalysts achieve current densities of 10 mA cm −2 at only 19.6 ± 0.1, 20.9 ± 0.1, and 21.0 ± 0.1 mV in alkaline freshwater, chemical wastewater, and seawater, respectively, while maintaining satisfied stability with minimal activity loss after 40,000 cycles. In situ experiments and theoretical calculations reveal that the ultra-low coordination of Pt, Ru, and Ni atoms creates numerous dangling bonds, which lower the water dissociation barrier and optimizing hydrogen adsorption. This research marks a notable advancement in the precise engineering of atomically dispersed multi-metallic centers in catalysts for energy-related applications.
研究领域:
催化
·
材料科学
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环境科学
·
能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Mengyao Luo,Longli Bo,Sining Huang,Haiguang Wang,Zhiyun Yang,Danjun Wang,Ying Yang,Zhe Li,Lu Wang
Adding polyethylene glycol (PEG) can lessen the shedding of coating and improve the dispersion of active particles for monolithic catalysts. In this study, a series of Cu-Mn-Ce-O x (P x )/TiO 2 (P x )/CH catalysts were prepared with different PEG molecular weights (P x , x = 200, 1000, and 2000) to explore the effect of P x addition on the structure and activity of the catalysts in microwave catalytic combustion of toluene. The research showed that P x addition (1 wt% dosage to titanium sol) to coating reduced the particle size of titanium sol and decreased the shedding rate of TiO 2 coating 0.9–0.93 %, and P x addition (3 wt% dosage to CH's water absorption) to active components further lessened the shedding rate of the catalysts 1.93–2.04 %. Under an initial toluene concentration of 1500 mg/m 3 and a gas hourly space velocity of 2260 h −1 , Cu-Mn-Ce-O x (P 1000 )/TiO 2 (P 1000 )/CH owned the highest catalytic activity and its complete removal temperature (T R100 ) and mineralization temperature (T M100 ) to toluene were 180℃ and 218℃, respectively, which were lower 33℃ and 16℃, 56℃ and 58℃ than Cu-Mn-Ce-O x /TiO 2 (P 1000 )/CH and Cu-Mn-Ce-O x /TiO 2 /CH catalysts separately, and its activity maintained steadily with toluene removal efficiencies of 99–91 % over 12 h. The improved activity is attributed to the uniform dispersion of active particles, larger specific surface area, and increased adsorbed oxygen, facilitated by pore-forming and steric-hindrance effects of P x . Electron transfer among Mn 4+ /Mn 3+ /Mn 2+ , Cu 2+ /Cu + , and Ce 4+ /Ce 3+ promoted the oxidation of toluene under microwave irradiation. Therefore, the research provides technological support for developing transition metals-based catalysts for industrial VOC waste gas treatment.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2020
·
IF 5.778
Zhao-Feng Yuan,Williamson Gustave,John Boyle,Raju Sekar,Jonathan Bridge,Yuxiang Ren,Xianjin Tang,Bin Guo,Zheng Chen
The sharp redox gradient at soil-water interfaces (SWI) plays a key role in controlling arsenic (As) translocation and transformation in paddy soils . When Eh drops, As is released to porewater from solid iron (Fe) and manganese (Mn) minerals and reduced to arsenite . However, the coupling or decoupling processes operating within the redox gradient at the SWI in flooded paddy soils remain poorly constrained due to the lack of direct evidence. In this paper, we reported the mm-scale mapping of Fe, As and other associated elements across the redox gradient in the SWI of five different paddy soils. The results showed a strong positive linear relationship between dissolved Fe, Mn, As, and phosphorus (P) in 4 out of the 5 paddy soils, indicating the general coupling of these elements. However, decoupling of Fe, Mn and As was observed in one of the paddy soils. In this soil, distinct releasing profiles of Mn, As and Fe were observed, and the releasing order followed the redox ladder. Further investigation of As species showed the ratio of arsenite to total As dropped from 100% to 75.5% and then kept stable along depth of the soil profile, which indicates a dynamic equilibrium between arsenite oxidization and arsenate reduction. This study provides direct evidence of multi-elements’ interaction along redox gradient of SWI in paddy soils.
研究领域:
土壤学
·
环境科学
✓ 已验证
DOI
PubMed
高影响因子
SOLID STATE IONICS
·
2021
·
IF 3.785
Yawen He,Zhongbin Ye,Mohamad Chamas,Moulay Tahar Sougrati,Pierre-Emmanuel Lippens
The silicon based composite Si/Cu-Zn(ox)/C was prepared by ball milling from Si microparticles , Cu-Zn nanopowder heated at air and carbon black. The composite is formed by Si submicrometer particles, Cu-rich Cu x Zn, CuO , ZnO and C nanoparticles . The two oxides are electrochemically active during the first discharge, improving the nanostructuration of the composite and providing Cu nanoparticles that enhance the electronic conductivity with Cu x Zn and C. The nanostructuration helps to buffer the volume variations due to Li-Si alloying reactions during cycling. The composite is further nanostructured during the first cycles as shown by XRD and electrochemical measurements. The material was tested as anode material for Li-ion batteries, providing a reversible capacity of 800 mAh.g −1 during 100 cycles at current of 300 mA.g −1 and a good rate capability. The reversible capacity is mainly due to Li-Si alloying reactions and is stable after few cycles while the solid electrolyte interphase is stabilized after about ten cycles as shown by electrochemical impedance spectroscopy .
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
WATER AIR AND SOIL POLLUTION
·
2026
·Vol. 237
·期 10
·572
·
IF 3.5
Zhang Jian,Wang Ningruo,Xie Xuewen,Liao Siyi,Zhong Biao,Feng Bo,Tian Chunxiang,Xu Yajun,Chen Yuhan,Xiao Jiewen
This study systematically evaluates the efficiency and mechanism of Mn–Co bimetallic oxides for peroxymonosulfate (PMS) activation to degrade bisphenol AF (BPAF). A series of spherical Mn a Co (1-a) O x catalysts were synthesized via a facile hydrothermal method. Among them, Mn 0.2 Co 0.8 O x exhibited the highest catalytic activity, outperforming other ratios. Under optimized conditions ([BPAF] = 5 mg/L, [PMS] = 0.2 mM, [Mn 0.2 Co 0.8 O x ] = 400 mg/L, pH = 7.85), the Mn 0.2 Co 0.8 O x /PMS system achieved 97.7% BPAF removal. Quenching tests and EPR spectroscopy confirmed SO 4 •⁻ and •OH as the predominant reactive oxygen species, with SO 4 •⁻ playing the dominant role. XPS and mechanism analysis indicated that the synergistic Co(III)/Co(II) and Mn(III)/Mn(II) redox cycles drive the efficient PMS activation and BPAF degradation.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF RARE EARTHS
·
2020
·
IF 3.104
Youchun Pan,Qijie Jin,Bingxu Lu,Yan Ding,Xin Xu,Yuesong Shen,Yanwei Zeng
MnCeO x /TiO 2 has been widely used in selective catalytic reduction (SCR) of NO x at low temperature. However, it is often poisoned in the presence of water vapor and sulfur dioxide . In this work, the promotion mechanism of Ba modification was investigated. Results show that the doped BaO reacts with CeO 2 and forms BaCeO 3 . This unique perovskite structure of BaCeO 3 significantly enhances NO oxidation and NH 3 activation of MnCeO x /TiO 2 catalyst so that the NO conversion and the resistances to SO 2 improve. It is found that Ba species obviously promotes the NO adsorption ability and improve the redox properties of MnCeO x /TiO 2 catalyst. While the acid properties of the catalyst are inhibited by Ba modification and among which Lewis acid sites are dominant for both MnCeO x /TiO 2 and MnCe(Ba)O x /TiO 2 catalysts. Furthermore, in situ DRIFT experiments reveal that the NO reduction upon MnCeO x /TiO 2 and MnCe(Ba)O x /TiO 2 catalysts follows both E-R and L-H mechanisms, in which L-H is preferred. Ba species enhances the formation of active nitrate species, which accelerates the NO reduction through L-H mechanism. It is interesting that although Ba species weakens the NH 3 adsorption, it induces the ammonia conversion to coordination ammonia, which in turn accelerates the catalytic reaction .
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2019
·Vol. 25
·期 68
·15586-15593
·
IF 5.16
Rengui Li,Yixuan Yang,Na Sun,Long Kuai
Development of Pt group metal-free catalysts for low-temperature CO oxidation remains critical. In this work, active and stable mesoporous Cu-Ce-O x solid solutions are prepared by using spray pyrolysis. The specific surface areas and pore volumes reach as high as 170 m 2 g −1 and 0.24 cm 3 g −1 , respectively. The results of CO oxidation study suggest that (1) the catalyst obtained by spray pyrolysis possesses much higher activity than those made by co-precipitation, sol-gel, and hydrothermal methods; (2) the optimal Cu 0.2 -Ce 0.8 -O x solid solution presents a reactivity over 28 times that of both single-component CuO and CeO 2 at 70 °C. Based on the study of pure-phase Cu-Ce-O x solid solutions by selective leaching of segregated CuO x species, the active center for CO oxidation is confirmed as the bimetallic Cu-Ce-O site, whereas the individual CuO x particles not only act as spectators but also block the active Cu-Ce-O sites. A low apparent activation energy of approximately 48 kJ mol −1 is detected for CO oxidation at the Cu-Ce-O site, making Cu-Ce-O x solid solutions able to present high activity at low temperature. Furthermore, the Cu-Ce-O x catalysts exhibit excellent stability and thermal tolerance toward CO oxidation. Graphical Pt-free CO oxidation : Well-shaped mesoporous Cu-Ce-O x solid solutions were produced for low-temperature CO oxidation by using a nitrate spray pyrolysis route, and a selective leaching strategy was adopted to remove the surface segregated CuO x species. The bimetallic Cu-Ce-O site was confirmed as the active center for CO oxidation, whereas the individually segregated CuO x species not only acted as spectators, but also blocked the active Cu-Ce-O sites (see scheme).
研究领域:
催化化学
·
材料科学
·
环境化学
·
能源化学
·
纳米材料
✓ 已验证
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2016
·
IF 4.712
Ru-Jia Yu,Wei Ma,Mao-Pan Peng,Zhi-Shan Bai,Yi-Tao Long
A novel redox-mediated chromogenic reaction was demonstrated based on the reaction between HAuCl 4 and 2,2-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS), which generate various color responses from red to green in the resulting solutions. Various redox substance could be used to mediate the reaction and trigger a distinct color response. We established a sensitive hydrogen peroxide colorimetric sensor based on the redox-mediated chromogenic reaction and depicted the application both in detection of enzyme and in an immunoassay . Combining the traditional chromogenic reagent with gold nanoparticles , our assay has the advantage in short response time (within three minutes), high sensitivity (10 −12 g mL −1 for HBsAg) and stability.
研究领域:
生物化学
·
医学检测
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）