Journal of the American Chemical Society
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2023
·
IF 15
Zhi-Zheng Wu,Xiao-Long Zhang,Peng-Peng Yang,Zhuang-Zhuang Niu,Fei-Yue Gao,Yu-Cai Zhang,Li-Ping Chi,Shu-Ping Sun,Jing-Wen DuanMu,Pu-Gan Lu,Ye-Cheng Li,Min-Rui Gao
Carbon–carbon coupling electrochemistry on a conventional copper (Cu) catalyst still undergoes low selectivity among many different multicarbon (C2+) chemicals, posing a grand challenge to achieve a single C2+ product. Here, we demonstrate a laser irradiation synthesis of a gerhardtite mineral, Cu2(OH)3NO3, as a catalyst precursor to make a Cu catalyst with abundant stacking faults under reducing conditions. Such structural perturbation modulates electronic microenvironments of Cu, leading to improved d-electron back-donation to the antibonding orbital of *CO intermediates and thus strengthening *CO adsorption. With increased *CO coverage on the defect-rich Cu, we report an acetate selectivity of 56 ± 2% (compared to 31 ± 1% for conventional Cu) and a partial current density of 222 ± 7 mA per square centimeter in CO electroreduction. When run at 400 mA per square centimeter for 40 h in a flow reactor, this catalyst produces 68.3 mmol of acetate throughout. This work highlights the value of a Cu-containing mineral phase in accessing suitable structures for improved selectivity to a single desired C2+ product.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Xing Yu,Jixiang Zhang,Nian Li,Yanping Song,Jun Kang,Shudong Zhang,Cui Liu,Zhao Li,Jingwen Pu,Na Hong,Min Xi,Zhenyang Wang
Combining of graphene with pseudocapacitance metal oxide is effective to construct supercapacitor electrode with high energy storage capacity. However, balancing the contradiction between high load of metal oxide and high stability of electrode is still challenging. Herein, a novel supercapacitor electrode composed of 3D graphene and manganese oxide is in-situ fabricated by laser carbonization of polyimide (PI) foam loaded with manganese acetate precursor. Due to the rich porous structure and super hygroscopicity of PI foam, high content manganese acetate is uniformly loaded into the network of PI foam. Under laser irradiation, PI foam is carbonized to form 3D porous graphene, while the generation of MnO-Mn 3 O 4 and its uniform loading on graphene is achieved synchronously. The obtained composite electrode exhibits a commercial-level mass loading up to 8 mg cm −2 , with a 48.6% weight ratio of MnO-Mn 3 O 4 . As a result, an ultra-high specific capacitance of 1525 mF cm −2 can be obtained for the composite electrode at the optimal doping concentration of 0.3 mol L − 1 . Notably, the composite electrode also exhibits excellent cycling stability of 94.75% retention rate after 6000 cycles. The maximum area specific capacitance of the micro supercapacitor with PVA/LiCl gel electrolyte is 410.19 mF cm −2 , the maximum energy density and power density are 82.04 μWh cm −2 and 400 μW cm −2 , respectively.
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CHINESE JOURNAL OF CATALYSIS
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2023
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IF 16.5
Hui Gao,Gong Zhang,Dongfang Cheng,Yongtao Wang,Jing Zhao,Xiaozhi Li,Xiaowei Du,Zhi-Jian Zhao,Tuo Wang,Peng Zhang,Jinlong Gong
Electrochemical CO 2 reduction is a sustainable method for producing multicarbon alcohols. However, the selectivity of alcohols is limited owing to the favorable side reaction to convert the key intermediate of *CH 2 CHO into ethylene. This study describes the design of a Cu electrocatalyst with abundant step sites to suppress the deoxygenation of *CH 2 CHO to ethylene, thereby promoting alcohol production. A Faradic efficiency of 40.5% and partial current density of 56.3 mA/cm 2 for alcohols are achieved. Moreover, the alcohols/C 2 H 4 ratio in the products reaches approximately 2.2. In-situ infrared spectrum characterizations and theoretical calculations reveal that the step sites facilitate C–C coupling and direct the reaction pathway to promote the formation of alcohols by inhibiting the cleavage of the C–O bond in *CH 2 CHO. Therefore, the proposed strategy is efficient for designing active sites to steer reaction pathways in CO 2 electroreductions and produce alcohols.
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Coatings
·
2023
·Vol. 13
·期 9
·1557
·
IF 3.4
Yan Gao,Xin Chen,Ping Xu,Jie Chen,Shihua Yu,Zhigang Liu,Xiaodan Zeng
A novel magnetic fluorescent nanoprobe (Fe3O4@ZnS@MPS(MFNPs)) was synthesized, which recognized and cooperated with Ag+ions, and a rapid method for detecting Ag+was established in solution. It was found by fluorescence spectroscopy analysis that the MFNPs could detect Ag+in PBS solution and, upon addition of Ag+ions, the fluorescence (FL) of MFNPs could be quenched significantly. The sensor has a low limit of detection (LOD) of 7.04 µM for Ag+. The results showed that MFNPs were extremely specific and sensitive for the quantitative detection of Ag+over a wide pH range. Then, the recognition mechanism between MFNPs and guest Ag+was explored via measures of infrared spectroscopy and electron microscopy. It was speculated that the oxygen atoms in the sulfonic acid group cooperated with Ag+to form a synergistic complexation. The assay was successfully used to determine the content of Ag+ in real samples.Keywords:magnetic fluorescent nanosensor;selective recognition;silver ion;3-sulfhydryl-1-propane sodium (MPS)
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Abubakar Yakubu Haruna,Yubo Luo,Zheng Ma,Wang Li,Haiqiang Liu,Xin Li,Qinghui Jiang,Junyou Yang
The thermoelectric performance of n-type Bi2Te3 needs further enhancement to match that of its p-type Bi2Te3 counterpart and should be considered for competitive applications. Combining Cu/Cl and multiscale additives (AgBiSe2) presents a suitable route for such enhancement. This is evidence of the enhanced thermoelectric performance of Bi1.995Cu0.005Te2.69Se0.33Cl0.03. Moreover, by incorporating 0.65 wt % AgBiSe2 (ABS) into Bi1.995Cu0.005Te2.69Se0.33Cl0.03, we further reduce its lattice thermal conductivity to ∼0.28 W m–1 K–1 at 353 K owing to the extra phonon scattering of multiscale ABS. Additionally, the Seebeck coefficient enhances (−183.89 μV K–1 at 353 K) owing to the matrix’s reduced carrier concentration caused by ABS. As a result, we achieve a high ZT of ∼1.25 (at 353 K) and a high ZTave of ∼1.12 at 300–433 K for Bi1.995Cu0.005Te2.69Se0.33Cl0.03 + 0.65 wt % ABS. This work provides a promising strategy for enhancing the thermoelectric performance of n-type Bi2Te3 through Cu/Cl doping and ABS incorporation.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Xin Liu,Peng Xu,Zhuoyu Yang,Pengfei Zhu,Jingwei Ma,Qiulai He,Baolin Hou
Zero-valent copper (Cu(0))-triggered hydrogen peroxide (Cu(0)/H 2 O 2 ) process was used to eliminate and mineralize contamination, while its oxidation efficacy was limited by the reaction of Cu(I) with O 2 . In this study, ferric ion (Fe(III)) was spiked into the Cu(0)/H 2 O 2 (Fe(III)/Cu(0)/H 2 O 2 ) system, and the degradation rate of paracetamol decreased from 24.9% to 95.4%. In the Fe(III)/Cu(0)/H 2 O 2 system, the reaction of Cu(0) and Cu(I) with Fe(III) expedited the conversion from Fe(III) to Fe(II). The reaction of Cu(I) with O 2 was weakened by the competition reaction between Cu(I) and Fe(III), promoting the generation of reactive oxygen species and increasing the utilization of Cu(0). The main reactive oxygen species for pH 4.0 was •OH and Fe(IV) with the contribution rate of •OH and Fe(IV) being 92.3% and 7.7%, but the dominant reactive oxygen species at pH 3.0 was only •OH in the Fe(III)/Cu(0)/H 2 O 2 process. Especially, the contribution of Fe(IV) rose and the contribution of •OH decreased, when the concentrations of 20–80 μmol/L Fe(III), 0.05–0.3 g/L Cu(0) and 50–300 μmol/L H 2 O 2 incremented. In the Fe(III)/Cu(0)/H 2 O 2 process.After we increased the pH of end solution to 7.0/7.5/8.0 and leaching, the total copper in reaction solution was under 6.4/3.3/1.5 μmol/L. In addition, Ni(II) (57.7%), Fe(II) (100%) and Mn(II) (72.4%) obviously enhanced the degradation of paracetamol in the Cu(0)/H 2 O 2 process.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2023
·Vol. 34
·期 23
·1-10
·
IF 2.8
Yuan Yulei,Zhang Minghui,Li Junjie,Liu Zhi-Quan
The application of wide bandgap semiconductor devices requires high-performance interconnect materials which have high thermal conductivity and high-temperature resistance. Among which, Cu nanoparticle paste sintering technology is regarded as an advanced alternative. However, Cu nanoparticles are easy to be oxidized, which needs an inert or vacuum atmosphere during the sintering process that restrict the practical application of Cu sintering technology. In this paper, a new type of Cu nanoparticle paste with antioxidation property was prepared by mixed commercial Cu nanoparticles (average diameter: 100 nm) treated by formic acid and reducing solvents containing 1-dodecanethiol. Based on the Cu nanoparticle paste, the pressure-assisted bonding at different bonding temperatures and times was carried out without using any protective atmosphere. A remarkable high shear strength of 55.06 MPa for Cu–Cu joints formed by sintering of Cu nanoparticle paste was achieved when sintered at 250 °C. The results of bonding experiment suggest that the proposed Cu nanoparticle paste has excellent antioxidation property and shows great application potential in high power electronic packaging.
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International Journal of Nanomedicine
·
2023
·
IF 8
Yan Zhou,Zekun Zhou,Xiaojuan Wu,Zefeng Wang,Wangdan Qi,Jing Yang,Liming Qing,Juyu Tang,Le Deng
Purpose We aimed to develop an oxidative-stress-activated palladium-copper nanozyme to reduce bacterial’s heat sensitivity by down-regulating heat shock proteins to overcome the shortcomings of conventional photothermal antimicrobial therapy and achieve mild photothermal bactericidal efficacy.Methods We first synthesized palladium-copper nanozymes (PC-NPs) by hydration and used transmission electron microscopy, X-ray diffraction, and Fourier transform infrared spectroscopy to demonstrate their successful preparation. Their photothermal therapy (PTT) and chemo-dynamic therapy (CDT) activities were then determined by a series of photothermal performance tests and peroxidase-like performance tests, and the destruction of heat shock proteins by reactive oxygen species (ROS) was verified at the protein level by Western Blotting tests, providing a basis for the effective bacteria-killing by the mild-temperature photothermal treatment subsequently applied. We also validated this promising programmed and controlled antimicrobial treatment with palladium-copper nanozymes by in vivo/in vitro antimicrobial assays. A hemolysis assay, MTT cytotoxicity test and histopathological analysis were also performed to assess the in vivo safety of PC-NPs.Results In the micro-acidic environment of bacterial infection, PC-NPs showed peroxidase-like activity that broke down the H2O2 at the wound into hydroxyl radicals and down-regulated bacterial heat shock proteins. The application of PC-NPs increased bacteria’s sensitivity to subsequent photothermal treatment, enabling the elimination of bacteria via mild photothermal treatment.Conclusion The programmed synergistic catalytic enhancement of CDT and mild photothermal therapy achieves the most efficient killing of bacteria and their biofilms, which brings future thinking in the relationship between heat shock proteins and oxidative stress damage in bacteria.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Peng Xu,Pengfei Zhu,Zhuoyu Yang,Xin Liu,Ruoxi Wu,Baolin Hou
The Cu 0 -stimulated PDS system, which produces reactive oxygen species (ROS) to decompose environmental pollutants, has been widely studied. Although Cu + is produced in the Cu 0 -stimulated PDS system, its susceptibility to disproportionate and easy oxidized by O 2 must be considered. To improve the utilization of Cu + , Cl − and Fe 3+ were considered for strengthening the Cu 0 -stimulated PDS process. With the addition of Cl − and Fe 3+ in the Cu 0 -stimulated PDS system (Cl − /Fe 3+ /Cu 0 /PDS system), the decomposition of tetracycline was greatly increased within 8 min. In the Cl − /Fe 3+ /Cu 0 /PDS system, Cl − limited the disproportionation reaction of Cu + by promoting Cu 0 and Cu 2+ reaction with Cl − and increased Cu + utilization rate. Fe 3+ promoted the recycling of Fe 2+ /Fe 3+ and contributed to reducing the invalid oxidation of Cu + by O 2 . Sulfate radical, reactive chlorine species and hydroxyl radical were generated in the Cl − /Fe 3+ /Cu 0 /PDS system. NO 3 − and SO 4 2− had no influence on decomposing tetracycline in the Cl − /Fe 3+ /Cu 0 /PDS system, but humic acid inhibited tetracycline decomposition. Moreover, the Cl − /Fe 3+ /Cu 0 /PDS system had great performance on the experimental water samples with the removal rate of tetracycline was higher than 80%. Furthermore, when the final solution pH was adjusted to 8.0, only 0.88 mg/L total dissolved copper remained after precipitation and filtering.
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PACKAGING TECHNOLOGY AND SCIENCE
·
2023
·Vol. 36
·期 11
·941-950
·
IF 2.6
Wenjiao Ge,Han Yu,Xiaohui Wang
Natural antioxidants are beneficial additives for active packaging due to their ability to resist oxidative damage. Polymeric micelles are effective in delivering natural antioxidants in aqueous environments. However, individual encapsulation of a single antioxidant may not be sufficient to meet the needs of modern food packaging. A dual natural antioxidant-loaded micellar system (i.e., vitamin E [VE] and curcumin [Cur]) was developed to achieve combined functionality and high loading concentration. Chitosan-graft-oleic acid (CSOA) micelles were employed as carriers to co-encapsulate VE and Cur through a facile ultrasound-assisted self-assembly method. The prepared VE and Cur co-loaded micelles (CSOA/VE/Cur) exhibited a uniform spherical structure with an average particle size of 210.6 nm and a zeta potential of +29.5 mV. Moreover, the co-encapsulation of VE and Cur showed a significant enhancement in both entrapment efficiency, loading capacity and stability as compared to the individual encapsulation of either VE or Cur. In addition, the CSOA/VE/Cur micelles showed improved antioxidant activity than free VE/Cur at the same concentrations, as evidenced by 2,2-diphenyl-1-picrylhydrazyl (DPPH) and ferric reducing antioxidant power (FRAP) assays. Moreover, the micellar materials were utilized to fabricate regenerated cellulose (RC) films with antioxidant properties, highlighting their potential as additives for antioxidant active packaging.
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MINERALS ENGINEERING
·
2023
·
IF 4.8
Xiaopeng Chi,Zihan Ye,Hao Wang,Wei Weng,Shuiping Zhong
The nature of copper slag flotation is unique due to the high temperature in the flotation pulp and high metallic copper content in the feed. Despite its great potential for valorizing slag, copper slag flotation remains challenging due to the deactivation of traditional dithiocarbonate (DTC) collectors (e.g., butyl xanthate) under high temperatures. DTC collectors also respond poorly to the metallic copper due to the difficulty in forming stable chemical adsorption. In this work, possible deactivation mechanisms of DTC collectors are proposed, i.e., decomposition, oxidation and thermal desorption. A novel furfuryl trithiocarbonate (FTTC) collector was designed and synthesized. Spectral characterization using FT-IR, H-NMR and ion trap MS confirmed the molecular structure of the synthesized collector and its decomposition, oxidation and polymerization products at 55 °C. The novel collector features high-temperature resistance and high metallic copper recovery, as revealed by the single mineral flotation experiments of chalcopyrite, pyrite and metallic copper at both 25 °C and 55 °C. The high collecting ability and selectivity of our collector were explained by E HOMO and E LUMO values using first-principles calculations. Our work provides guidance for the design of collectors exhibiting high-temperature resistance for copper slag flotation, aims at constituting a meaningful contribution for unlocking potential copper resources in copper slag.
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TRIBOLOGY INTERNATIONAL
·
2023
·
IF 6.2
Hongming Wei,Gangwen Feng,Xiaoya Li,Wenyi Zhan,Feiyang Li,Yanzhang Dai,Jianpeng Zou
Cu/graphite composites are widely used in various fields as friction materials . However, their tribological properties are limited by the inadequate wettability between Cu and graphite and the insufficient strength of the Cu matrix. To strengthen Cu/graphite composites and improve their interface bonding, this investigation employed Cr 2 AlC to modify Cu/graphite composites fabricated by spark plasma sintering (SPS). The microstructure, interface characteristics, and tribological properties of the composites were thoroughly examined. The results show that the composites exhibit favorable tribological properties, which improved with the increase in sintering temperature . Specifically, as the sintering temperature increases from 800 °C to 980 °C, the friction coefficient of the composites decreases from 0.170 to 0.138, while the wear rate decreases from 9.92 × 10 −7 mm 3 /N·m to 1.86 × 10 −7 mm 3 /N·m.
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