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
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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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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
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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
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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
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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
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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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Journal of Materials Chemistry A
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2025
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IF 9.5
Zhijian Chen,Zhenghui Ma,Wenlin Yang,Guoli Fan,Baoming Ren,Feng Li
Due to the high energy barrier of C-C coupling and the intense competition from by-products, achieving superior ethylene selectivity in electrochemical CO2 reduction reaction (eCO2RR) remains challenging. Herein, we reported a distinctive Cu-based electrocatalyst fabricated from a three-dimensional (3D) tentacle-like Cu2(OH)2CO3 precursor. After electrochemical activation, abundant surface structural hydroxyls chemically bonded to Cu+ species (Cu+-OH structures) formed on the resulting Cu-based electrocatalyst. Such structural hydroxyl-rich Cu-based catalyst exhibited excellent eCO2RR performance, with a Faradaic efficiency (FE) of 43.7% for ethylene (partial current density up to 130.6 mA·cm-2) and a FE of ~70% for C2+ products at -1.5 V vs RHE in a flow cell, far exceeding those over the hydroxyl-deficient Cu-based one. By combining operando spectroscopic analysis with density functional theory calculations, it was unveiled that inherent surface Cu+-OH structures over Cu-based electrocatalysts could result in the electron loss of neighboring active Cu0 sites, which was favorable for the creation of crucial *COH and *OCCOH intermediates and thus the formation of ethylene product. Consequently, dual reaction pathways for the eCO2RR based on both key *COH and *CHO intermediates coexisting on the Cu-based electrocatalyst with abundant Cu+-OH structures powerfully boosted electrochemical CO2 reduction to produce ethylene. This work presents an innovative strategy for the construction of Cu-based electrocatalyst rich in structural hydroxyls and highlights the crucial role of inherent Cu+-OH structures in switching the formation of intermediates to boost ethylene production in the eCO2RR.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Hongman Sun,Yuanyuan Wen,Yaqian Li,Rong Fan,Yonglian Lu,Chao Feng,Hao Liu,Youhe Wang,Zhipeng Ma,Yu Zhang,Rose Amal,Zifeng Yan
Ag@Cu 2 O tandem catalysts is effective to improve the selectivity of hydrocarbons in CO 2 RR, where Ag core generates *CO intermediates, which migrate to Cu 2+ /Cu + interface, promoting proton transfer and C-C coupling forming *OCCHO. However, Cu + crucial for C-C coupling exhibits instability under reductive conditions. Herein, we used Ag@Cu 2 O tandem catalysts as a sacrificial template to synthesize Ag@Cu 2 O@Cu-BDC (BDC = 1,4-benzenedicarboxylic acid) tandem catalysts through an in-situ conversion strategy, which can not only introduce Cu 2+ , but also stabilize Cu + by forming a Cu-BDC MOF shell. In addition, by adjusting the amount of sacrificial template, the controllable regulation of Cu 2+ and Cu + content was successfully achieved, forming a Cu 2+ /Cu + valence state fluctuation buffer zone. It is found that this modulation not only significantly improve the selectivity towards hydrocarbons (CH 4 +C 2 H 4 ), but also enables the regulation of the reaction pathway, thereby allowing for fine-tuning of product selectivity. Notably, the Ag@Cu 2 O@Cu-BDC-5 tandem catalyst with a lower Cu 2+ /Cu + ratio demonstrated superior CH 4 selectivity (59.3 %), while the Ag@Cu 2 O@Cu-BDC-10 tandem catalyst with a higher Cu 2 ⁺/Cu + ratio achieved dominant C 2 H 4 production (43.0 %) under applied potential of −1.4 V vs. RHE for 20 h. This is attributed to Cu 2+ sites facilitated *CHO generation, while Cu + sites promoted C-C coupling as evidenced by the in-situ infrared and DFT calculations. Additionally, this study demonstrated the existence of a tandem catalysts that could increase the CO coverage on Cu sites, ensuring the full utilization of Cu + and Cu 2+ sites to further enhance product selectivity and reduce the overpotential for optimal product generation.
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CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Xianlong Lu,Lili Wang,Xueyang Zhao,Binbin Pan,Zhendong Li,Xiangfei Du,Shihan Zhang,Fan Dong,Bangwei Deng
Copper (Cu)-based catalysts show significant potential for producing high value-added C 2+ products in electrocatalytic CO 2 /CO reduction reactions (CO (2) RR). However, the structural reconfiguration during operation poses substantial challenges in identifying the intrinsic catalytic active site, especially under similar mass transport conditions. Herein, three typical and commercial Cu-based catalysts (Cu, CuO, and Cu 2 O) are chosen as representatives to elucidate the structure-activity relationship of CORR in the membrane electrode assembly electrolyzer. Notably, only the Cu catalyst demonstrates the most suppression of hydrogen evolution reaction, thus achieving the highest FE of 86.7% for C 2+ products at a current density of 500 mA cm –2 and maintaining a stable electrolysis over 110 h at a current of 200 mA cm –2 . The influence of chemical valence state of Cu, electrochemical surface area, and local pH were firstly investigated and ruled out for the significant FE differences. Finally, based on the structure analysis from high resolution transmission electron microscope, OH – adsorption, in situ infrared spectroscopy and density functional theory calculations, it is suggested that the asymmetric C-C coupling ( via *CHO and *CO) is the most probable reaction pathway for forming C 2+ products, with Cu (100)-dominant grain boundaries (GBs) being the most favorable active sites. These findings provide deeper insights into the synergistic relationship between crystal facets and GBs in electrocatalytic systems.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Chunyi Ye,Yang Yang,Shujing Chen,Chunhua Liu,Xiao-Qing Sun,Danni Liu,Jiujun Zhang,Jing-Li Luo,Xian-Zhu Fu
Hydrogen (H 2 ) is a promising green alternative fuel; however, the widespread adoption of H 2 production technologies is limited by high energy consumption and significant carbon emissions. Here, we have developed a bipolar H 2 production electrolyzer that purifies wastewater and produces H 2 with ultra-low energy consumption by combining the formaldehyde 1-electron oxidation reaction (FOR-1) at the anode and the hydrogen evolution reaction (HER) at the cathode. The electroless Cu electrode exhibits high selectivity and activity for the 1-electron pathway of formaldehyde oxidation (i.e., FOR-1), enabling the anodic conversion of formaldehyde into valuable H 2 and formate. This facilitates the treatment of toxic formaldehyde waste while doubling H 2 production efficiency of the electrolyzer. Unlike conventional water electrolysis, the formaldehyde-water electrolyzer demonstrates a cell voltage reduction of 1.49 V at 10 mA/cm 2 . At 100 mA/cm 2 , the energy consumption is reduced to only 25 % of that in conventional systems, even with the use of a nickel foam cathode. Moreover, formaldehyde in wastewater is fully degraded within 50 min, highlighting its practical application potential.
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