JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Lijun Yue,Wanjun Zhao,Jinfang Li,Ruifang Wu,Yongzhao Wang,Hongxi Zhang,Yongxiang Zhao
The impact of Indium (In) doping upon the catalytic performance of Pd-Cu/Al 2 O 3 for carbon monoxide preferential oxidation (CO-PROX) in hydrogen (H 2 ) rich atmosphere at low temperature has been studied. A series of catalysts with extremely low palladium (Pd) loading (0.06 wt%) are synthesized by the facile co-impregnation method. When the In/copper (Cu) atomic ratio equals 0.25, Pd-Cu-In 0.25 /Al 2 O 3 can keep 40% CO conversion and 100% carbon dioxide (CO 2 ) selectivity at least 120 min at 30 °C, which is significantly superior to the catalytic performance of Pd-Cu/Al 2 O 3 . The elaborate characterization findings reveal that the added In species to Pd-Cu/Al 2 O 3 causes Indium oxide (In 2 O 3 ) to generate, which produces the interaction of In 2 O 3 with Pd-Cu/Al 2 O 3 , further promoting the dispersion of copper chloride hydroxide (Cu 2 Cl(OH) 3 ). Moreover, the modification of In facilitates the re-oxidation of Pd 0 to Pd + through reducing the formation of palladium hydride (PdH x ) during the CO-PROX reaction. Meanwhile, the addition of In leads to the decrease of Cu + electron cloud density, making it easier to be oxidized to Cu 2+ . Collectively, the easy re-oxidation of Pd 0 and Cu + is favorable to fulfill the Wacker cycle between Pd and Cu species, thus improving the catalytic performance for CO-PROX.
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Journal of Energy Chemistry
·
2024
·
IF 14
Haotian Duan,Wenyang Li,Lixiu Ran,Fulong Zhu,Tianxiang Li,Ming Miao,Wen-jin Yin,Xin Wang,Yongzhu Fu
The conversion of carbon dioxide to ethylene by electrochemical reduction (CO 2 RR) provides a new strategy for achieving carbon dioxide conversion. However, copper-based catalysts have the disadvantages of unsatisfactory selectivity and low current density, which limit the potential CO 2 RR industrial expansion. Researches have verified that the real reaction sites at the catalyst surface often undergo reconstruction during the reaction, therefore, understanding and utilizing this phenomenon is crucial for improving catalytic performance. In this work, we introduced additional Ag component into Cu@Ag/C tandem catalyst by in-situ electrochemical reconstruction of Cu 2 CO 3 (OH) 2 /AgCl/C precursor. This electro-reduced catalyst exhibits a C 2 H 4 Faradaic efficiency of 50.41% in H-cell, and 58.03% in the flow cell, surpassing the counterparts of pure Cu and Ag, as well as the Cu-Ag homolog with separated interface. Moreover, it also provides a long-term stability of 21 h with the ethylene Faraday efficiency (FE) over 50%. The appropriate amount of Ag dopant into the Cu catalyst changes the electronic structure of Cu surface by the electron transfer from Cu to Ag, which distinctly enhances the binding energy of CO 2 on the catalyst. Meanwhile, in-situ Raman results and theoretical calculation reveal that the introduction of silver increases the number of active sites and improves the coverage of *CO intermediate, thereby accelerating the kinetics of C–C coupling and reducing its energy barrier. The combination of cascade catalytic strategy and in-situ electroreduction interface provides potential applications for future artificial carbon balance.
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ACS Catalysis
·
2024
·
IF 11.3
Yuheng Ma,Yu Zhang,Guanshun Xie,Zhaohui Huang,Linfen Peng,Changqiang Yu,Xiuqiang Xie,Shuanglin Qu,Nan Zhang
Doping engineering has enabled the construction of homogeneous and abundant atomic-level catalytic sites for photocatalytic CO2 reduction with improved selectivity for the target product. However, little is known about the effect of the spatial position of the heteroatoms on the photocatalytic activity of the semiconductors toward CO2 reduction. Herein, uniform Cu doping into the bulk phase of hollow CdS cubes (HCC) and Cu doping onto the surface of HCC, denoted as Cu/HCC and HCC@Cu, respectively, are prepared by tuning the introduction order of Cu sources. Experimental analysis shows that the introduction of Cu by both methods can promote the separation and migration of photoinduced charge carriers in CdS. Notably, Cu doping onto the surface of CdS in HCC@Cu leads to much better proton reduction to H2 production performance but lower CO2 reduction efficiency as compared to bare CdS. In sharp contrast, Cu doping into the bulk phase of CdS enhances the CO2-to-CO conversion while mitigating H2 evolution. This should be ascribed to the smaller overpotential of Cu/HCC in the CO2 saturated system than that in the Ar system. In addition, doping Cu atoms into the bulk phase of CdS shifts the d band center of Cu/HCC upward to near the Fermi energy level, which promotes the adsorption and activation of CO2 on CdS. These results indicate that the photoelectrons with a prolonged lifetime in Cu/HCC preferably reduce CO2 molecules rather than protons. The density functional theory (DFT) calculation results show that the introduction of Cu heteroatoms can promote the desorption of CO*, and the adaptable sulfur vacancies (Vs) produced by in situ doping techniques can stimulate the formation of CO* intermediates, resulting in the high performance of photocatalytic CO2 reduction to CO. This work reveals the effect of different heteroatom doping locations on the catalytic activity and will provide a reference for the design of efficient photocatalysts with atomic-level fine structure.
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Journal of Environmental Sciences
·
2024
·
IF 5.9
Xuan Liang,Jin Zhang,Juntai Tian,Zenghua Xie,Yue Liu,Peng Liu,Daiqi Ye
Herein, three supported catalysts, CuO/Al 2 O 3 , CeO 2 /Al 2 O 3 , and CuO-CeO 2 /Al 2 O 3 , were synthesized by the convenient impregnation method to reveal the effect of CeO 2 addition on catalytic performance and reaction mechanism for toluene oxidation. Compared with CuO/Al 2 O 3 , the T 50 and T 90 (the temperatures at 50% and 90% toluene conversion, respectively) of CuO-CeO 2 /Al 2 O 3 were reduced by 33 and 39 °C, respectively. N 2 adsorption-desorption experiment, XRD, SEM, EDS mapping, Raman, EPR, H 2 -TPR, O 2 -TPD, XPS, NH 3 -TPD, Toluene-TPD, and in-situ DRIFTS were conducted to characterize these catalysts. The excellent catalytic performance of CuO-CeO 2 /Al 2 O 3 could be attributed to its strong copper-cerium interaction and high oxygen vacancies concentration. Moreover, in-situ DRIFTS proved that CuO-CeO 2 /Al 2 O 3 promoted the conversion of toluene to benzoate and accelerated the deep degradation path of toluene. This work provided valuable insights into the development of efficient and economical catalysts for volatile organic compounds.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Keying Hua,Yongjia Shi,Miaomiao Tang,Xiangyu Zuo,Jun Gao,Xia Zhang
Water-based lubricants are essential in the field of tribology , and the application of nanoparticles as additives in water-based lubricants shows promise and significant practical importance. In this study, water-soluble Cu nanoparticles modified with methoxypolyethyleneglycol xanthate long-chain polymers were fabricated by a in-situ surface modification method. The tribological behavior of the Cu nanoparticles synthesized as additives in a water-PEG system was evaluated using a universal micro-tribotester. It was found that the synthesized nanoparticles could be stably dispersed in the water-PEG system and could enhance the tribological properties and load-carrying capacity of the system significantly. For example, the coefficient of friction could be reduced to 0.052, and the P B value increased to 588 N when the Cu nanoparticles were added at a mass fraction of 1.5 %. This was mainly attributed to the formation of a boundary lubrication film consisting of Cu, Fe 2 O 3 , Fe 2 (SO 4 ) 3 , and FeS throughout the entire friction process. The boundary film effectively prevents direct contact between the friction surfaces, thereby improving the tribological properties. The incorporation of Cu nanoparticles as additives into commercial cutting fluids resulted in a lower coefficient of friction and significantly enhanced the extreme pressure performance of the cutting fluids, demonstrating promising application prospects.
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Materials Today Communications
·
2025
·
IF 4.5
Yi Zhang,Hao Wang,Man Li,Xinhao Sun,Yan Zhang,Zhifeng Wang,Chunling Qin
This work successfully synthesizes a new type of multi-layered flexible hybrid electrode (Cu/Ni(OH) 2 /np-Ni) composing of bimetallic components, hierarchical porous structure and outstanding glucose electrocatalytic performance. The synthesis strategy includes a facile two-step approach, i.e. the Ni(OH) 2 nanolayer in-situ grows on a nanoporous Ni (np-Ni) network (Ni(OH) 2 /np-Ni) via deionized water immersion and then the metallic Cu dendrites are uniformly deposited on Ni(OH) 2 /np-Ni. Moreover, due to the hierarchical porous structure as well as synergetic effect of Ni(OH) 2 and Cu dual electroactive components, the Cu/Ni(OH) 2 /np-Ni hybrid electrode electrodeposited with 1 min delivers wider linear range of 18 mM and higher sensitivity of 1.629 mA mM −1 cm −2 . The electrode possesses excellent interference immunity, reproducibility as well as long-time stability. In addition, the mechanism of electrochemical sensors for detecting glucose under alkaline conditions is briefly introduced. Accordingly, the flexible Cu/Ni(OH) 2 /np-Ni electrode material shows promise for further development as a contender for wearable glucose sensors.
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Nano Research
·
2024
·
IF 9.5
Li Jing,Jing Chuanyong,Wang Jin
Electrocatalytic CO 2 reduction to CH 4 remains challenging due to multi-electron transfer and intermediates adsorption. Herein, we synthesized electrocatalysts by growing Ni-Cu alloy structure on nitrogen-doped carbon nanotubes (Ni x Cu y -NCNT) for electrocatalytic CO 2 reduction reaction (CO 2 RR) via hydrothermal method followed by pyrolysis. The optimized Ni 1 Cu 1 -NCNT demonstrated a superior CO 2 RR performance, achieving 99.7% \(\text{FE}_{\text{CH}_{4}}\) (FE = Faradaic efficiency) and 11.54 mA • cm −2 current density at −1.2 V vs. reversible hydrogen electrode (RHE), which outperformed single metal counterparts. Its outstanding performance was due to the electrons transferred from Cu to Ni and Ni-Cu alloy shifted the d-band center toward the Fermi level, which was more conducive to the intermediate formation. In situ electrochemical attenuated total reflection (EC-ATR) and density functional theory (DFT) calculations revealed the appearance of *CHO intermediate and the pathway during the CO 2 RR process. The design of the bimetallic electrocatalyst in this study provides a new perspective for the highly selective reduction of CO 2 .
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ACS Applied Nano Materials
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2024
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IF 5.3
Yaqi Qu,Hualiang An,Xinqiang Zhao,Yanji Wang
The development of a sustainable catalytic system for optimizing the use of noble metals (NMs) plays a crucial role in expanding the application of NMs. In this paper, we synthesized a series of core–shell nanoparticles (NPs) with metal Cu as a core and ultrathin NM M (M = Pt, Pd, Rh, Ru, Ir, and Au) as a shell. Cu–M NPs were fabricated via a one-pot method, which involved a two-step process of Cu nucleating first at a low temperature and then NMs nucleating and growing on the Cu core at a high temperature later. For Pd precursor salt with a lower decomposition temperature, introducing trioctylphosphine (TOP) to enable the in situ formation of Pd-TOP complex was pivotal to obtaining Cu–Pd. X-ray diffraction, high-angle annular dark-field scanning transmission electron microscopy, and energy-dispersive X-ray spectroscopy-mapping characterizations highlight the core–shell NPs with an ultrathin shell. The catalytic performance of the Cu–M NPs was investigated by using selective hydrogenation of nitrobenzene as a probe reaction. Among them, Cu–Rh demonstrated enhanced activity toward nitrobenzene hydrogenation to aniline with a TOF value as high as 2847 h–1. While a part of aniline would undergo excessive hydrogenation to cyclohexylamine over a pure Rh NP catalyst. Valence band spectra measurement and density functional theory calculations both prove that the activity modulation is principally governed by the charge transfer. The introduction of Cu core downshifts the d-band center of the Rh shell, weakens the adsorption of aniline, and thereby terminates the further reduction of aniline. The synthesis of Cu–M NPs can not only reduce the dosage of NMs but also present the potential for activity control by adjusting the properties of the shell metals. These core–shell NPs provide considerable promise for terminating the reaction to the intermediate product in consecutive hydrogenation reactions.
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MICROCHEMICAL JOURNAL
·
2024
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IF 4.9
Xu Liu,Peide An,Yide Han,Hao Meng,Xia Zhang
Cu-based nanozyme shows good oxidase-like activities due to the changeable states of Cu(II) and Cu(I), which are proven to be effective in the electron transfer in the redox process. Herein, the self-made MOF-818 with more Cu(II) loading was synthesized through a modified two-steps hydrothermal routes, which was then used as a sacrificial precursor to construct copper/zirconium composite oxides nanozymes (CN-MOF-818). The pyrolysis temperature was varied to obtain the best enzyme-like activities of the resulting CN-MOF-818. The laccase-like and catecholase-like activities were evaluated by using the oxidation of the mixture of 4-aminoantipyrine (4-AAP) and 2,4-dichlorophenol (2,4-DP), and 3,5-Di- tert -butylcatechol (3,5-DTBC) respectively. The enzyme-like activities were optimized through altering the catalytic conditions, and the corresponding enzyme catalytic kinetics including K m and V max were also determined. The enzyme-like mechanism of the CN-MOF-818 were also discussed based on EPR technique and the in-situ FT-IR analyses. In comparison with the pristine MOF-818 and the other reported Cu-based mimics, the as-prepared CN-MOF-818 exhibits the higher oxidase mimetic activities. These CN-MOF-818 can also be employed to detect the epinephrine with a low detection limit of 1.63 μM.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yurui Xu,Xiao Liu,Minghui Jiang,Ning Li,Mingxue Su,Xin Du,Shiyu Li,Lei Lu,Suping Cui
Electrochemical carbon dioxide reduction reaction (ECO 2 RR) to produce high value-added products is a promising and effective strategy for closing the artificial carbon cycle and achieving sustainable development of resource. However, catalyst structural reorganization and agglomeration caused by the reduction process will reduce the catalytic performance. In this study, a carbon nitrogen shell with cupper-doped (CNCu shell) catalyst was prepared using silicon dioxide (SiO 2 ) as a template. The selectivity of the catalyst was controlled by precisely adjusting the form of Cu doping in the catalyst. When doped as single-atoms (CNCu 2.5 ), the catalyst exhibited a Faraday efficiency of up to 85 % for formate at −0.9 V versus reversible hydrogen electrode (vs. RHE). In contrast, when both Cu clusters and single-atoms coexisted (CNCu 25 ), the catalyst favored multi-carbon products, with a Faraday efficiency of 45 % for ethanol and 23 % for acetic acid. Density functional theory (DFT) calculations revealed the key mechanism for the difference in catalyst selectivity between the two doping forms. Cu single-atoms provided suitable binding energy to HCOO*, which increased the rate of CO 2 conversion to formate, while the combination of Cu clusters and single-atoms increased the adsorption of HCOO*, raising the rate-determining step energy of the formate pathway, which favored multi-carbon products. This study fundamentally revealed how different doping forms of metals affect catalyst selectivity, providing new insights and strategies for developing superior metal–carbon–nitrogen (M C N) catalysts.
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ELECTROCHIMICA ACTA
·
2025
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IF 5.6
Juan Li,Jinggao Wu,Chang Ming Li
Dual hetero paired single atomic catalyst (DHAC, CoCu@CN) was one-pot synthesized by a facile green method and applied as a nanozyme for the detection of H 2 O 2 . Both experimental results and theoretical calculations discover that the hetero-paired DAC realizes stronger adsorption energy and a bridge adsorption of H 2 O 2 for simultaneous 2-electron transfer, thereby offering much higher electrocatalytic activity and larger catalytic current than that of single Co atom and single Cu catalyst alone toward H 2 O 2 reduction. The CoCu@CN H 2 O 2 sensor demonstrates a wide linear detection range (0.654–7379.454 μM) and low limit of detection (LOD) of H 2 O 2 (0.047 μM), and is used successfully to in-site detect intracellular H 2 O 2 released from living cells, ensuring its practical applications in life science and medical diagnosis. This work not only discloses a scientific insight for the enhancement mechanism of the dual single heteroatomic catalyst, but also demonstrates an avenue to synthesize more efficient dual single heteroatomic catalyst for potential broad applications in energy conversion and/or sensing applications.
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Nano Research
·
2018
·Vol. 11
·期 3
·1379-1388
·
IF 7.994
Liu Xiao-Yuan,Zhang Guozhen,Chen Hao,Li Haowen,Jiang Jun,Long Yi-Tao,Ning Zhijun
The development of photocatalysts that can effectively harvest visible light is essential for advances in high-efficiency solar-driven hydrogen generation. Herein, we synthesized water soluble CuInS 2 (CIS) and Cu-In-Zn-S (CIZS) quantum dots (QDs) by using one-pot aqueous method. The CIZS QDs are well passivated by glutathione ligands and are highly stable in aqueous conditions. We subsequently applied these QDs as a light harvesting material for photocatalytic hydrogen generation. Unlike most small band gap materials that show extremely low efficiency, these new QDs display remarkable energy conversion efficiency in the visible and near-infrared regions. The external quantum efficiency at 650 nm is ∼1.5%, which, to the best of our knowledge, is the highest value achieved until now in the near-infrared region.
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