Catalysis Science & Technology
·
2022
·Vol. 12
·期 20
·6155-6162
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IF 6.177
Lizi Shi,Huimin Liu,Shangbo Ning,Jinhua Ye
Photothermal catalysis is a promising strategy for converting CO2 into high value-added chemical feedstocks. Its current major challenges lie in improving CO2 conversion efficiency and product selectivity. In this work, a series of Cu/TiO2 core–shell catalysts were prepared using the hard template method. The Cu10/TiO2 catalyst exhibited excellent performance for the photothermal conversion of CO2 to CO in the presence of H2 under Xe lamp irradiation (CO2 conversion, 30.6%; CO selectivity, ∼100%; CO maximum yield, 87.1 mmol h−1 gcat−1). Results indicated that the Cu/TiO2 catalyst has a good photo-to-thermal conversion ability based on the significant LSPR effect, and the existence of hot electrons makes the reaction follow the carbonate pathway efficiently. This article successfully achieves efficient CO2 reduction under inexpensive and non-toxic conditions. In addition, it also provides unique insights into the study of the LSPR effect in the field of photothermal catalysis.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Nan Xin,Guihua Tang,Tian Lan,Yifei Li,Jiawei Kou,Min Zhang,Xin Zhao,Yinan Nie
Two-dimensional (2D) layered transitional metal dichalcogenides (TMDCs) semiconductors like MoS 2 have been predicted to be promising thermoelectric (TE) materials due to their high carrier mobility. However, the TE performance of MoS 2 film is severely hindered by the high in-plane thermal conductivity. In this work, based on reversing grain orientation reducing in-plane thermal conductivity, Cu doping is used to increase the carrier concentration for optimization of electrical properties. The Cu-doped MoS 2 films have prepared by magnetron sputtering (MS) combined with post-sulfurization chemical vapor deposition (CVD). The composition, structure, thermal and electrical properties were systematically investigated by experiment and DFT calculation. Results indicate that Cu doping may slightly reduce the Seebeck coefficient of MoS 2 film, but effectively narrow the band gap and improve the carrier concentration, thus improving the electrical performance. In addition, MS combined with CVD method can effectively increase the degree of grain misorientation, making the in-plane thermal conductivity of Cu-doped MoS 2 film much lower. Combined with the above optimization, a promising maximum ZT value among TMDCs 0.137 at 425 K was obtained in Cu 6 -MoS 2 film. This study provides a new strategy to synchronously regulate the thermal and electrical properties of TMDCs films to improve their thermoelectric performances.
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ENERGY & FUELS
·
2022
·
IF 4.654
Xuesong Shan,Keru Song,Fengyue Shi,Dongyu Zhao
Copper nanoparticles are uniformly supported on acidified carbon nanotubes (CNTs/Cu NPs) by a mild liquid-phase reduction method without surfactants or bridging molecules. The surface of copper nanoparticles is smooth without impurities. Then, polystyrene (PS) microspheres are prepared by emulsion polymerization and composited with CNTs/Cu NPs (CNTs/Cu NPs/PS). Nanocopper/carbon nanotubes as the core and polyaniline as the shell were prepared via situ polymerization as a core–shell structure (PANI@CNTs/Cu NPs/PS). At a high temperature, the PS cracks and eliminates materials, forming porous structures, and the polyaniline is carbonized, realizing nitrogen doping of the material (NCMP). The results indicated that the acidified carbon nanotubes played a crucial role in the synthesis procedure, achieving consistent growth of copper on carbon nanotubes. The size of evenly dispersed copper nanoparticles is about 5–15 nm. When NCMP is applied as an electrode material, it demonstrates excellent electrochemical performance as a high-performance supercapacitor.
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高影响因子
FUEL
·
2022
·
IF 8.035
Chaohe Zheng,Mingze Su,Haibo Zhao
As the kinetic influencing factors were not considered properly in the previous studies, the obtained activation energies of copper oxidation were discrepantly ranging from 15.0 kJ/mol to 100.0 kJ/mol. The gas diffusion in the crucible and sample layer, the surface reaction and the defect diffusion of copper cations all have an impact on the conversion process of copper oxidation samples. Using the high diameter-height ratio crucible in our self-made TGA could effectively eliminate the gas diffusion in the crucible and reduce the error of the kinetic tests. Based on the previous four-step oxidation mechanism, the kinetic parameters of copper oxidation are identified using a grain-scale kinetic model, coupling with a defect transport model. The potential kinetic impact factors including the particle polydispersity, gas diffusion, defect diffusion, surface reaction and particle sintering are adequately considered in this work. First, it is found that the copper oxidation is not dominated by the defect diffusion in the solid product layer, but governed by the surface reaction in the gas–solid interface. The copper oxidation is likely to be adsorption-limited during the surface reaction in the gas–solid interface, and the intrinsic activation energy is identified as 48.0 kJ/mol. The particle-scale model is then performed to investigate the impact of physical properties of oxygen carrier particles. It can significantly accelerate the conversion rate of copper oxidation by means of decreasing the particle size and increasing the porosity. However, it is not advisable to decrease the grain size too much when preparing the oxygen carriers, for this will only increase diffusion resistance inside the particle for small grain. Finally, it can be found that in most conditions of the air reactor, Cu-based oxygen carrier with the grain size of 220–300 nm exhibits the best oxidation performance.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Yaru Xi,Zuoyi Xiao,Hui Lv,Haodong Sun,Shangru Zhai,Qingda An
Copper oxide (CuO) and copper (Cu) have been viewed as the prospective pseudocapacitive electrode materials for supercapacitors. Nevertheless, the poor electron transfer capacity, loading amount, and cycling stability limit their wide applications, which can be addressed by developing the CuO based heterojunction on conductive carbons. Here, a CuO/Cu@C comprising CuO/Cu nanoflowers and chitosan-derived N -doped porous carbon was compounded by simple mechanical mixing, freeze-drying, and carbonization. The composite heated at 700 °C exhibited a high specific capacitance of 2479F/g at 0.5 A/g and excellent cycling stability with capacitance retention of 82.43 % after 10 000 charge–discharge cycles. In addition, the asymmetric supercapacitor (ASC), i.e., CuO/Cu@C-700//AC assembled by CuO/Cu@C (as a positive electrode) and activated carbon (AC, as a negative electrode) displayed a great energy density of 76.87 W h kg −1 at 374.5 W kg −1 and kept as high as 25.83 W h kg −1 even at 14998 W kg −1 . Our work provides a new pathway to preparing transition metal oxide-based electrode materials with distinguished electrochemical performances.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 40
·19542-19554
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IF 3.925
Xiaoqing Wang,Binhe Zhao,Zimeng Xu,Haosong Chen,Tong Ye,Jing Zhang,Xinyue Zhang,Aoqi Ji,Jionghui Li,Chunhua Xiong
A series of novel resin-based MOF composites Co-MOF@D113-N (N = 1, 6) were prepared using 2-methylimidazole, cobalt acetate and D113 resin, through the layer-by-layer self-assembly method. The Co-MOF presented an amorphous form with the inducement of resin groups and the loading capacity increased with the number of self-assembled layers. The strong anchoring effect between Co and N effectively improved the thermal stability of the composites. The adsorption experiments showed that the adsorption capacity of the Co-MOF@D113-6 resin for Cu(II) increased with temperature in the range of 283–303 K. The adsorption capacity of Co-MOF@D113-6 for Cu(II) increased under the synergistic effect of MOFs and D113. The maximum adsorption capacity of Co-MOF@D113-6 was 273.88 mg g−1. The fitting results showed that the adsorption of Cu(II) by the Co-MOF@D113-6 conformed to the pseudo-second-order kinetic model dominated by chemisorption, and also conformed to the preferential Freundlich adsorption isotherm model. A low cost resin carrier combined with a high efficiency MOF composite adsorption material provided high efficiency and low consumption for promising development.
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高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yaoyu Zhang,Yuxiong Wang,Yue Liu,Huimin Xu,Zhongbiao Wu
Aiming at the coexistence of pollutants in the actual industrial process, the catalytic oxidation of acetonitrile and ethyl acetate mixture on the Cu–Ce/ZSM–5 catalyst was studied. The mutual inhibition effect during catalytic removal of acetonitrile and ethyl acetate mixture was observed. Acetonitrile showed a more obvious inhibitory effect on the conversion of ethyl acetate, and the introduction of ethyl acetate reduced the N 2 selectivity of acetonitrile oxidation. The simulation results demonstrated acetonitrile could be preferentially adsorbed on Cu center of the catalyst surface, leading to significant inhibition of the initial conversion of ethyl acetate. In addition, the coexistence of ethyl acetate would weaken the hydrolysis of acetonitrile to generate carboxylic acid and –NH x species. As such, no enough adsorbed NH x species could be used to reduce the NO x produced by excessive oxidation of acetonitrile, resulting in a decreased in N 2 selectivity. This study could provide reference on the application of catalysts for cyanide–containing waste gas degradation.
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MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 9
·1-10
·
IF 6.408
Zhou Xuemei,Qi Yuji,Tang Yulian,Gao Hui,Lv Li,Lei Xingyu,Hu Lei,Yan Zhengquan
To enhance the peroxidase-like performance and its application in detection of toxic o -aminophenol ( o -AP), a kind of bimetal Cu–Zn oxide-based mesoporous nanosphere (Cu 2/3 Zn 1/3 O PNPs) was constructed under microwave-radiation conditions. Its mesoporous microstructure and peroxidase-like catalytic activity were investigated in detail. The results showed that Cu 2/3 Zn 1/3 O PNPs possessed a high specific surface area of 34.89 m 2 g −1 and a well-distributed mesoporous size of approximate 6.07 nm, which endowed the superior peroxidase-like performance. The material catalyzes the oxidization of 3,3′,5,5′-tetramethylbenzidine (TMB) with K m / V max of 0.104 mM/3.79 × 10 −8 M·s −1 in the presence of H 2 O 2 . Especially o -AP could exclusively deteriorate the characteristic UV–Vis absorbance intensity at 653 nm ( A 653 ) of the Cu 2/3 Zn 1/3 O PNPs-TMB-H 2 O 2 system with obvious color change from blue to colorless. Under the optimal conditions, the effect of some interfering substances was low and the limit of detection (LOD) for o -AP was 1.65 × 10 −8 mol/L (S/N = 3). When applied to the colorimetric detection of o -AP in practice, the recovery was between 96.1 and 107.2% with R.S.D. less than 2.04%. The mechanism of synergic-enhancement peroxidase-mimic activity of Cu 2/3 Zn 1/3 O PNPs and its exclusive colorimetric response to o -AP were proposed as well. Graphical abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Pei Shen,Tiansheng Yang,Qichang Li,Zhi Chen,Yonglong Wang,Yunlei Fu,Jun Wan,Zexing Wu,Lei Wang
Developing efficient and stable catalysts for electrocatalytic hydrogen evolution reaction (HER) with low overpotential is the key point to realizing large-scale hydrogen commercialization. Herein, Ru doped amorphous hollow copper hydroxide nanowires on copper foam (Ru-Cu(OH) x /CF) is prepared by surface chemical oxidization and following solvothermal process. The hollow 3D nanowire structure can provide abundant accessibility active sites, promote electrolyte in filtration and facilitate gas diffusion in the process of the electrochemical reaction. Then, the as-synthesized Ru-Cu(OH) x /CF electrocatalyst exhibits impressive electrocatalytic performance for HER with 45, 80 and 50 mV to drive 10 mA cm −2 in 1.0 M KOH, 1.0 M phosphate-buffered saline (PBS) and 0.5 M H 2 SO 4 , respectively, with remarkable long-term stability. Moreover, sustainable energies can power the two-electrode setup with amounts of hydrogen generation. The strategy may be particularly beneficial to explore simple synthesis and high-performance catalysts for HER.
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Nanoscale
·
2022
·Vol. 14
·期 36
·13248-13260
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IF 8.307
Xin Huang,Haitao Li,Yin Zhang,Ruifang Wu,Lijun Ban,Lin Xi,Zhifang Yin,Jian Peng,Yongxiang Zhao,Li Fang
In conventional thermocatalytic reactions under a reducing atmosphere, stabilization of the active Cu+ component and inhibition of over-reduction into metallic Cu0 are extremely challenging. In this study, Au@Cu2O core–shell nano-catalysts with different Cu2O shell thicknesses were synthesized, and the effect of the Au nano-core on Cu+ stability under a reducing atmosphere and the catalytic performance of Cu+ in the ethynylation of formaldehyde were investigated. The Au nano-core facilitates Cu2O dispersion and leads to an increase of 0.2–0.5 eV in electron binding energies of Cu2O and Cu2C2 in the range of 27–55 nm, attributed to the long-range electromagnetic effect of Au NPs. Specifically, active Cu+ centers exhibit high stability under a reducing atmosphere due to the long-range electromagnetic effect of the Au nano-core. In the ethynylation of formaldehyde as a probe reaction, Cu+/(Cu0 + Cu+) on Au@Cu2O catalysts remained at 88–91%. The catalytic performance in the ethynylation of formaldehyde revealed that the introduction of an Au nano-core into Cu-based catalysts increased the TOF from 0.37 to 0.7 h−1, and decreased the activation energy from 42.6 to 38.1 kJ mol−1. Additionally, the Cu+/(Cu0 + Cu+) ratios and the catalytic performance in the ethynylation of formaldehyde (BD yield = 65%, BD selectivity = 95%) on Au@Cu2O catalysts remained constant after nine cycles, while pure Cu2O readily deactivated due to the dramatically reduced Cu+/(Cu0 + Cu+) ratios and carbyne deposition. In summary, Cu+ in Cu-based catalysts showed high catalytic activity and stability during the ethynylation of formaldehyde due to the long-range electromagnetic effect of the Au nano-core.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 37
·17767-17775
·
IF 3.925
Ji-Ping Jia,Yu-Lu Zhang,Jin-Yu Gou,Yi-Xuan Zhang,Yu-Ke Dai,Hong-Hua Ge,Yu-Zeng Zhao,Xin-Jing Meng
A Ti/SnO2–Sb–Cu–Zn electrode was prepared for the electrocatalytic oxidation of Acid Red 18 (AR18). The addition of Zn to the coating results in smaller surface cracks and greater roughness. When Cu and Zn coexist, high-index crystal planes are generated on smaller-sized grains formed on the coating surface, which allows the coating surface to adsorb oxygen. Sb5+ and the adjacent Cu2+–Zn2+ on the surface of the Cu–Zn co-doped coating are the advantageous active sites for adsorbed oxygen. The electrode exhibits a larger electrochemically active surface area and smaller electrochemical reaction resistance. The appearance of high-index crystal planes is beneficial to improve the electrocatalytic activity of the electrode, although the oxygen evolution potential of the electrode is not greatly improved. Cu–Zn co-doping produces synergistic mineralisation and enhances the ability to degrade AR18, and ˙OH is the main active species. During the thermal decomposition of the coating, Zn induces Cu to form more active sites on the high-index crystal planes of SnO2, a phenomenon that may be responsible for the synergistic production of more reactive oxygen species on the electrode surface.
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RSC Advances
·
2022
·Vol. 12
·期 34
·21875-21884
·
IF 4.036
Ruimeng Sun,Ruijuan Lv,Yang Zhang,Ting Du,Yuhan Li,Lixia Chen,Yanfei Qi
The catalytic properties of bimetallic nanoparticles have been widely studied by researchers in many fields. In this paper, core–shell Cu/Au nanoparticles (Cu/Au NPs) were synthesized by a simple and mild one-pot method, and their peroxidase activity was proved by catalyzing the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) with color change to blue. The change of solution color and absorbance strongly depends on the concentration of H2O2, so it can be used for direct detection of H2O2 and indirect detection of glucose. What's more, GSH can efficiently react with the hydroxyl radicals from H2O2 catalyzed by core–shell Cu/Au NPs to inhibit the production of ox-TMB. Thus, the concentration of GSH can be determined by the decrease in the absorbance of the solution at 652 nm. The results showed that our proposed strategy had good detection range and detection limit for the detection of glucose and GSH. This method has been used in the detection of practical samples and has great application potential in environmental monitoring and clinical diagnosis.
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