iScience
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2022
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IF 6.107
Zhicong Lu,Peng Zhang,Chun Hu,Fan Li
Summary Persulfate-based nonradical oxidation processes are appealing in water treatment for the efficient and selective degradation of trace contaminants in complex water matrices. However, there is still lacking of systematic understanding of the relationship between multiple nonradical pathways and the active sites of catalyst. Herein, a single-atom Cu catalyst with saturated Cu-N 4 sites on a carbon substrate (SA-Cu-NC) was constructed to activate peroxymonosulfate (PMS), which exhibited high catalytic performance and selectivity for pollutant degradation in different water conditions. Combined with the results of density functional theory (DFT) calculations, the electron-rich area around Cu site and the electron-poor area around C site in the saturated Cu-N 4 configuration could efficiently adsorb and activate PMS, which promoted pollutant degradation through the oxidation of singlet oxygen ( 1 O 2 ) and electron transfer process, respectively. This study advances the understanding of the saturated coordination structure of metals and the superiority of multiple nonradical pathways in wastewater treatment.
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PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2021
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IF 9.229
Hongjing Wang,Qiqi Mao,Tianlun Ren,Tongqing Zhou,Kai Deng,Ziqiang Wang,Xiaonian Li,You Xu,Liang Wang
Achieving high efficiency in nitrate (NO3–) to ammonia (NH3) electrocatalysis requires the exploration of advanced electrocatalysts with a well-designed composition and architecture. In this work, a facile one-step hydrothermal approach was developed for the construction of novel Cu/oxygen vacancy-rich Cu-Mn3O4 heterostructured ultrathin nanosheet arrays on Cu foam (Cu/Cu-Mn3O4 NSAs/CF). Two-dimensional ultrathin nanosheet arrays could increase the exposure of catalytically active centers, and the heterogeneous nanointerface and oxygen vacancies synergistically improve the nitrate-to-ammonia activity over the active centers. Due to the desirable compositional and structural advantages, the Cu/Cu-Mn3O4 NSAs/CF demonstrated excellent performance for the electrocatalytic nitrate reduction to ammonia with high ammonia selectivity (87.6%) and Faradic efficiency (92.4%).
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PubMed
高影响因子
CHEMOSPHERE
·
2021
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IF 7.086
Xiaoping Liu,Yunbo Zhai,Guangli Liu,Xiangmin Liu,Bei Wang,Zhexian Wang,Ya Zhu,Yuwei Fan,Haoran Shi,Min Xu
Without extra adjustment of pH, the effects of cupric ions (Cu(II)) and hydrogen peroxide (H 2 O 2 ) alone or in combination on sludge dewatering were studied. It showed good dewatering capability after treated by Cu(II) and Cu(II)/H 2 O 2 , which indicated by the capillary suction times (CST) decreased from 120.8 ± 4.7 s (control) to about 40 s, and the water content (Wc) of sludge cake dropped by about 10%. The results showed that the extracellular polymeric substances (EPS) were destroyed, which characterized by a significant decrease in the biopolymers’ concentrations in tightly-bound EPS. Meanwhile, more rough and porous microstructures and higher zeta potentials were obtained after conditioned. Based on the changes of physicochemical properties of sludge, the variations of EPS, and the identification of reactive species, two distinct mechanisms of improved sludge dewatering were postulated. As for Cu(II) treatment, it was mainly due to the surface charge neutralization, strong cytotoxicity of Cu(I) produced by intracellular reduction of Cu(II), and pH decline caused by Cu(II) hydrolysis that improved sludge dewatering performance, which could be noted as a “non-radical pathway”. When in combination with H 2 O 2 , hydroxyl radicals (·OH) produced by Cu(II)-catalyzed Fenton-like process played a dominant role in degrading sludge flocs and EPS, which could be regarded as a “radical pathway”.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Zhen Zhong,Min Li,Jinghao Fu,Yuexin Wang,Yaseen Muhammad,Sihan Li,Jiaxing Wang,Zhongxing Zhao,Zhenxia Zhao
Cu 2 O/MIL(Fe/Cu) composite was fabricated via an in-situ Cu-bridging strategy to enhance interfacial synergistic effect of photo-Fenton catalysis for thiacloprid (TCL) degradation. Characterization results showed that: (1) Cu 2 O was proved to grow on the surface of MIL(Fe/Cu) in Cu 2 O/MIL(Fe/Cu) composite and display a high BET surface area of 1553 m 2 /g; (2) Cu 2 O/MIL(Fe/Cu) reduced band gap from 2.5 to 1.3 eV and extended absorption from UV to visible region; (3) Cu-bridge was proved to promote the intimate interface between Cu 2 O and MIL(Fe/Cu), which accelerated charge transferred and shortened the binding gap and the reaction pathway from photo-induced electrons to Fenton-generated radicals. As a result, this boosted the redox reaction of Fe 2+ /Fe 3+ and promoted the reversible degree of this catalytic redox ability of MIL(Fe). Catalytic performance exhibited that (1) Cu 2 O/MIL(Fe/Cu) showed a fast kinetics (2–40 times faster than the state-of-the-art catalysts) and ultra-high mineralization (82.3% within 80 min) for TCL degradation; (2) Cu 2 O/MIL(Fe/Cu) showed a promising cycling stability due to improved charge transfer ability that could protect Cu 2 O from photo-corrosion during photo-Fenton reaction; (3) The catalytic performance of Cu 2 O/MIL(Fe/Cu) was characterized and seven photocatalytic intermediates were identified by both HPLC/MS and Surface Enhanced Raman Spectroscopy. The cyanoimino group in TCL was proved for the first time to be attacked primarily. Moreover, among all the detected intermediates, thiazolidin-2-amine (P6) was found to be the most stable intermediate to be degraded, and it can directly influence the TOC determination during photodegradation process.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
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IF 4.2
Ning Ma,Xitao Wang,Xuemei Liu,Ningyan Li,Yuan Liu
Inhibiting the sintering of Cu-based catalysts for CO2 reverse water–gas shift (RWGS) reaction is still a great challenge. Herein, Cu–Al spinel supported on Al2O3 was prepared by a surface solid reaction and used as a precursor to obtain Cu particles with high dispersions and high stabilities. Due to the high dispersions of Cu cations in Cu–Al spinel, strong chemical interactions between Cu particles and newly generated Al2O3, and the isolation effects of Al2O3 particles, Cu particles derived from Cu–Al spinel exhibited smaller sizes after H2 reduction, excellent activities, and 300 h stabilities for RWGS reactions. However, Cu particles obtained from the supported CuO precursor showed much larger particle sizes (>70 nm) and inferior activities and stabilities for CO2 reverse water–gas shift reaction. This study made a successful attempt to enhance the activities and stabilities of Cu-based catalysts through changing the oxide precursor.
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ACS Catalysis
·
2023
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IF 12.9
Yuxue Yue,Saisai Wang,Qi Zhou,Bolin Wang,Chunxiao Jin,Renqin Chang,Liqi Wan,Zhiyan Pan,Yihan Zhu,Jia Zhao,Xiaonian Li
It remains challenging to achieve nanoparticles with uniform size and dispersion or single atoms with identical coordination structure, although various methods have been developed to synthesize carbon-supported nanostructured catalysts. Typically, in the synthesis of vinyl chloride (VCM) by acetylene hydrochlorination, a limited understanding of the optimal architecture for carbon-supported Cu catalysts at the nanoscale greatly restrains their further development and application. To achieve this, Cu single-atom (Cu-O3P) with identical coordination environments and Cu/Cu3P nanoparticles with uniform size were tailored via advanced carbothermal shock method, and their catalytic structure–activity relationships were explored in the acetylene hydrochlorination reaction. In detail, a platform of nanostructured copper catalysts was constructed by the precursor-assisted carbothermal shock method, and the relationship between the coupling structure and electron properties of copper sites and their catalytic performance is correlated. Finally, we derived quantitative activity and stability descriptors that account for the d-orbital coupling and competitive adsorption effects observed in acetylene hydrochlorination. This work provides a precise and versatile approach for designing well-defined carbon-supported metal nanocatalysts and regulating their catalytic performance.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Yanjie Han,Zhijia Zhu,Chunyan Hu,Jian Zheng,Baojiang Liu,Wei Wang
In this study, a novel three-dimensional, flower-like Cu-BiOCl/Bi 2 S 3 photocatalyst was synthesized using a two-step calcination and hydrothermal method , aiming at the efficient removal of tetracycline (TC). Through comprehensive characterization techniques, it was discerned that the incorporation of Cu ions extended the light absorption range of BiOCl. Additionally, the formation of a heterojunction significantly enhanced the separation efficiency of space charge. The unique three-dimensional flower-like architecture of the Cu-BiOCl/Bi 2 S 3 photocatalyst augments its surface area exposure and consequently, the density of active sites. This catalyst exhibited a remarkable degradation rate of approximately 95% for TC under visible light irradiation. This performance exhibits a notable enhancement over the degradation rates of BiOCl and Bi 2 S 3 , which are approximately 39% and 53% respectively, surpassing them by factors of 2.39 and 1.78. Electron spin resonance (ESR) analysis coupled with free radical trapping experiments pinpointed superoxide radicals (•O 2 - ) and photogenerated holes (h + ) as the pivotal active species orchestrating the photocatalytic degradation. Concludingly, a possible TC degradation pathway was proposed based on the intermediates generated during the photocatalytic reaction as detected by Liquid Chromatograph Mass Spectrometer (LC-MS) and Three-Dimension Excitation Emission Matrix (3D EEM).
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2019
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IF 6.393
Mingxia Jiao,Yun Li,Yuxiu Jia,Zhen Yang,Xiliang Luo
Non-cadimum photoluminescent I−III−VI semiconductor nanocrystals have attracted increasing attention due to their low toxicity, extraordinary optical and electronic properties. Herein, water-soluble quaternary Cu-In-Zn-S quantum dots (CIZS QDs) with tunable emission from 535 nm to 645 nm were successfully synthesized via ecofriendly one-pot aqueous method. The full width at half-maximum (FWHM) of the emissions are about 68 nm–88 nm, which are rather narrow among Cu-based semiconductors and preferred to facilitate improving color purity. The photoluminescence of water-soluble QDs was enhanced by ZnS coating with the absolute quantum yield (QY) up to 30.8%. Further, a novel fluorescent sensor for Cu 2+ detection was developed based on the alteration of intrinsic optical properties of the CIZS/ZnS QDs after cation exchange at room temperature within 10 min, presenting a linear range of 0.020–20 μM and a detection limit down to 6.7 nM. Mechanism studies revealed that the QDs served as the template for cation exchange, through UV–vis absorption and fluorescence spectra in combination with the chemical composition and time-resolved photoluminescence decay analysis. Ions interference experiments demonstrated the good selectivity of the QDs towards Cu 2+ and the sensor showed comparable accuracy to ICP-AES method as well as good performance in real sample detection, manifesting the reliability of the current strategy for sensing Cu 2+ mildly and rapidly.
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CATALYSIS TODAY
·
2018
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IF 4.667
Xianghui Li,Yingnan Zhao,Huawang Zhao,Mengke Liu,Yuhan Ma,Xin Yong,Hong Chen,Yongdan Li
Two kinds of Cu-SAPO-34 catalysts, prepared with a one-pot technique using Cu- tetraethylenepentamine as co-template and an ion-exchange method, were hydrothermally treated at 750 °C for at least 16 h. The migration of Cu species during hydrothermal treatment and the corresponding effect on the selective catalytic reduction (SCR) of NO x were examined and characterized. A certain amount of CuO exists outside and inner the crystallites in the as prepared ion-exchanged sample, whereas copper is mainly atomically dispersed in the one-pot sample existing as isolated Cu 2+ . After hydrothermal treatment for 16 h, the amount of the inner nanosized CuO in the ion-exchanged sample reduced and the copper disperses to form more isolated Cu 2+ . However, surface CuO particles increase at the sacrifice of isolated Cu 2+ with extending the hydrothermal treatment to 24 h. Aggregation of Cu 2+ species also happens during the aging treatment over the one-pot prepared sample where the initial Cu is atomically dispersed as isolated Cu 2+ . The increase of the amount of the isolated Cu 2+ enhances the low-temperature (< 350 °C) performance. However, the increase of the amount of surface CuO particles in the aged samples promotes the nonselective NH 3 oxidation reaction in the high temperature range and results in the lowering of the SCR activity by limiting NH 3 supply.
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MATERIALS LETTERS
·
2019
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IF 3.019
Kai Xu,Xiaohong Chen,Honglei Zhou,Liming Bi,Shaoli Fu,Wei Li,Xinkuan Liu,Fengcang Ma,Ke Zhang,Ping Liu
CNTs/Cu-Al 2 O 3 composite powders were successfully synthesized by in situ CVD using Cu-Al 2 O 3 composite powders obtained by internal oxidation of Cu-Al alloy powders. The multi-walled CNTs are obtained without agglomeration and stand on the surface of the composite powders. One end of the CNTs is well bound to matrix. The Cu nanoparticle was the catalyst for the growth of CNTs on the composite powders and Al 2 O 3 on the surface of the Cu-Al 2 O 3 powder plays a key role in the growth process.
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JOURNAL OF MATERIALS PROCESSING TECHNOLOGY
·
2024
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IF 6.7
Jianbo Xin,Yue Gao,Chenghao Zhang,Le Yang,Sushi Liu,Ke Li,Minghao Zhou,Yang Liu,Jing Zhang,William Cai
Copper (Cu) particle sintering is widely regarded as one of the most ideal interconnect technologies for wide band gap semiconductors owing to its potential for low-temperature curing while withstanding a higher working temperature. Nevertheless, the strict requirements for sintering conditions and high costs limit the widespread application of Cu sintering technology. In this paper, a simple vehicle was introduced into Cu paste formulation to achieve an effective sinter bonding even using commercially available sub-micron or even micrometer Cu particles (C-Cu particles) with the in-situ generation of composite Cu particles. This innovative vehicle comprises Cu salt, a combination of capping agents and reducing agents. The addition of the hybrid capping agent binds Cu atoms to the surface of the C-Cu particles and allows the generated Cu particles (G-Cu particles) produced from the vehicle to grow on their surface, resulting in the in-situ generation of composite Cu particles. Based on the in-situ generated composite Cu particles, sintering experiments were conducted at designated temperatures (200 °C, 225 °C, 250 °C) for various durations (3 min, 5 min, 10 min) in a N 2 atmosphere under different pressures (10 MPa, 15 MPa, 20 MPa). A reliable Cu sintered joint with a high shear strength of 41.3 MPa can be achieved at a low temperature (200 °C) using 500 nm C-Cu particles. Moreover, the joints sintered with large size (>3 μm) particles at 250 °C could also reach 43.3 MPa. The in-situ generated composite Cu particles accomplish the transformation of low-energy interfaces of C-Cu/C-Cu to high-energy interfaces of G-Cu/G-Cu, which in turn facilitates low-temperature sintered connection of C-Cu particles and reliable sintered joints formed of large size C-Cu particles. These findings improve the feasibility of Cu sinter bonding in practical applications.
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Journal of Materials Chemistry A
·
2024
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IF 10.7
Yunshuo Wu,Haiqiang Wang,Zhongbiao Wu
The development of catalysts with high-density interfacial sites is crucial for enhancing catalytic performance. However, the efficient construction of interfacial sites remains a significant challenge. In this study, we introduced a ligand-regulated co-precipitation synthesis strategy to fabricate a Cu@ZnO1-x/Al2O3 catalyst. The catalyst possesses high-density partially-reduced ZnO1-x-Cu interfacial sites and exhibits enhanced activity for CO2 hydrogenation to methanol. The methanol space-time yield (STY) of the Cu@ZnO1-x/Al2O3 was 3.8 times higher than that of the commercial Cu/ZnO/Al2O3 after 14 h continuous reaction. Molecular dynamics (MD) simulations and in situ Raman spectroscopy indicated that Cu‒X‒Zn linkage ligands formed in the precursor solution during hydrothermal treatment facilitated zinc-malachite formation during co-precipitation, which promoted Cu-ZnO interface formation during H2 reduction. Moreover, density functional theory (DFT) calculations confirmed partially-reduced ZnO1-x-Cu interfaces were more active via the formate pathway. This work reveals a novel and robust route for designing catalysts with high-density interfacial sites, shedding light on catalyst development.
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