JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Qiaohong Su,Qingcui Liu,Pengyue Wang,Juan Ding,Jiulin Wang,Yudai Huang
High overpotential and low stability are major challenges for hydrogen evolution reaction (HER)/oxygen evolution reaction (OER). Tuning the electronic structure of catalysts is regarded as a core strategy to enhance catalytic activity. Herein, we report CuO x /Cu nanorod skeleton supported Ru doped cobalt oxide/nitrogen-doped carbon nanocomposites (Ru-CoO/NC/CuO x /Cu, denoted as RCUF) as bifunctional catalysis. The one-dimensional/three-dimensional (1D/3D) nanostructure and defect-rich amorphous/crystalline phases of RCUF facilitates active site exposure and electron transport. Experimental characterization and density functional theory (DFT) calculation results indicate that Ru doping can optimize the electronic structure, which accelerates the water dissociation process and reduces the Gibbs free energy of the reaction intermediates. As expected, the optimal RCUF-900 exhibits low overpotential (25/205 mV at 10 mA cm −2 ) and high stability (100/100 h) for HER/OER. RCUF-900 has low voltage (1.54 V at 10 mA cm −2 ) and high stability (100 h) for overall water splitting. This work provides new insights into the design of advanced catalysts for overall water splitting.
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ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Zhibin Zhang,Lei Wang,Xixian Yang,Mengyuan Chu,Liyun Huang,Jiayi Fan,Wucheng Xie,Defei Liu,Wenbing Yuan,Yue Situ
The electroreduction of CO2 to formate is of significant interest due to its potential for sustainable fuel and chemical production. Hollow fiber electrodes, which integrate gas diffusion and catalytic layers, offer structural advantages. These advantages enhance gas–solid–liquid-phase reactions, making them particularly beneficial for CO2 electroreduction. This work reports a copper–bismuth alloy hollow fiber with a nanostructured surface, designed with specific metal ratios and transformed into a sulfur surface-modified copper–bismuth alloy hollow fiber (Cu7S4–CuBi HF) electrode with nanoflower structures. CO2-penetration mode enhances formate current density and Faradaic Efficiency (FE) while suppressing the hydrogen evolution reaction (HER), due to the fiber’s unique gas transport. The nanoflower morphology increases the electrochemical active surface area, boosting current densities. This design achieved a formate FE of 91.27% at −0.9 V vs RHE and a current density of 80.12 mA cm–2, outperforming many existing Cu@Bi electrocatalysts. This success is due to the innovative surface design and the distinct structural features of the hollow fiber electrodes.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2024
·
IF 1.5
Zhou Lu-Wei,Chen Kai-Wei,Dai Xiao-Jun,Qiao Tai-Fei,Liu Hong-Yu,Lu Ji-Gen,Wang Peng,Gong Chun-Hui,Deng Shao-Gang,Xia Ming,Ni Fei,Tang Guo-Min,Zhang Yong-Bing,Yang Yi
Cu/Cu 2 O-modified activated carbon composites (Cu/Cu 2 O@AC) were synthesized via an one-step solvothermal method. The characterization results indicated that copper was uniformly dispersed on the surface of AC as nano-sized Cu 0 and Cu(I), which allowed Cu/Cu 2 O to make full contact with I − . The high specific surface area of Cu/Cu 2 O@AC and the affinity of Cu + for I − led to the equilibrium adsorption capacity within forty minutes. Additionally, the removal of trace I − (300 μg L −1 ) at pH = 3 by Cu/Cu 2 O@AC reached 96.4%. This work provides a promising application for the inexpensive and efficient capture of trace iodine from medical wastewater. Graphical abstract We synthesized Cu/Cu 2 O@AC composites for adsorption of iodide ions in solution.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Xiang Zhang,Weihang Li,Jin Zhang,Haoshen Zhou,Miao Zhong
Electrochemical nitrate (NO 3 − ) reduction offers a promising route for ammonia (NH 3 ) synthesis from industrial wastewater using renewable energy. However, achieving selective and active NO 3 − to NH 3 conversion at low potentials remains challenging due to complex multi-electron transfer processes and competing reactions. Herein, we tackle this challenge by developing a cascade catalysis approach using synergistic active sites at Cu-Fe 2 O 3 interfaces, significantly reducing the NO 3 − to NH 3 at a low onset potential to about +0.4 V RHE . Specifically, Cu optimizes *NO 3 adsorption, facilitating NO 3 − to nitrite (NO 2 − ) conversion, while adjacent Fe species in Fe 2 O 3 promote the subsequent NO 2 − reduction to NH 3 with favorable *NO 2 adsorption. Electrochemical operating experiments, in situ Raman spectroscopy, and in situ infrared spectroscopy consolidate this improved onset potential and reduction kinetics via cascade catalysis. An NH 3 partial current density of ~423 mA cm −2 and an NH 3 Faradaic efficiency (FE NH3 ) of 99.4% were achieved at −0.6 V RHE , with a maximum NH 3 production rate of 2.71 mmol h −1 cm −2 at −0.8 V RHE . Remarkably, the half-cell energy efficiency exceeded 35% at −0.27 V RHE (80% i R corrected), maintaining an FE NH3 above 90% across a wide range of NO 3 − concentrations (0.05−1 mol L −1 ). Using 15 N isotopic tracing, we confirmed NO 3 − as the sole nitrogen source and attained a 98% NO 3 − removal efficiency. The catalyst exhibit stability over 106-h of continuous operation without noticeable degradation. This work highlights distinctive active sites in Cu-Fe 2 O 3 for promoting the cascade NO 3 − to NO 2 − and NO 2 − to NH 3 electrolysis at industrial relevant current densities.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Siyuan Luo,Haiyuan Zou,Renji Zheng,Shimao Deng,Xuezhen Feng,Wenfei Wei,Ranhao Wang,Ze Li,Wei Xu,Lele Duan,Hong Chen
Selective electrochemical reduction of CO 2 /CO to high-valuable C 2+ products is of great importance to alleviate the global warming and energy crisis problems, while the selective production of C 2 is severely limited by the C C coupling pathway on the catalyst interface. Herein, by employing a Cu + /Cu 2+ charge-ordered metal-organic framework (MOF) material (denoted to be Cu4BHT) as a CO electroreduction catalyst, a high acetate selectivity of 50.3% at 0.7 V versus reversible hydrogen electrode (RHE) has been achieved. An in-depth mechanism study reveals that the charge-ordered Cu + /Cu 2+ pair on Cu4BHT interface favors the C O bond activation, C C coupling, and proton-coupled electron transfer dynamics, which results in the selective formation of C 2+ products. This work illustrates the critical role of employing charge-ordered Cu + /Cu 2+ catalytic site pair for C C coupling, which paves the way for designing highly selective catalysts to promote the formation of the C 2 products.
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CATALYSIS COMMUNICATIONS
·
2024
·
IF 3.4
Yu Sun,Jinxing Mi,Liang Li,Shuxiu Yu,Shixiong Yuan,Guimin Wang,Jianjun Chen,Junhua Li
The unique ability of Cu + to enhance C-C coupling makes it important in the field of CO 2 reduction reaction (CO 2 RR) over Cu-based catalyst, while Cu + is very prone to deactivation. Hereby, we propose a simple and feasible stabilization strategy to stabilize Cu + species through reducing Cu-Mg-Al hydrotalcite by adding ascorbic acid, which owns stable product selectivity in a span of 6 h at −0.95 V vs.RHE. Characterization results show that the excellent stability is promoted by the heterostructure of Cu 2 O and hydrotalcite with retained Cu + species, which derives from Cu 2 O and slow down the rapid reduction of Cu + to Cu 0 .
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IEEE TRANSACTIONS ON NUCLEAR SCIENCE
·
2024
·
IF 1.9
Wanting Gui,Lu Yao,Xunsheng Zhou,Qi Wu,Chao Li,Shi Zhang,Yunfeng Zhan,Cai Lin Wang
Ag-based metal halide scintillators have recently attracted significant interest for X-ray imaging due to their high light yield and ultra-fast decay lifetime. These properties are advantageous for thermal neutron detection, yet their application in this area have not been thoroughly explored. In this article, we investigate the properties of Cu-doped Cs
2
AgI
3
metal halide scintillators for X-ray imaging and thermal neutron detection. A simple synthesis process was employed to produce Cu-doped Cs
2
AgI
3
scintillators. The as-prepared Cu-doped Cs
2
AgI
3
exhibited intense green emission with a photoluminescence quantum yield (PLQY) of 55 ± 2.7%. Cu-doped Cs
2
AgI
3
/PVDF plastic scintillation screen has been prepared and achieved a resolution of 5 lp/mm under X-ray radiation. A composite consisting of
6
LiF, Cu-doped Cs
2
AgI
3
, and Poly (methyl methacrylate) (PMMA) was utilized for thermal neutron detection, achieving a light yield of about 12,526±9 photons/thermal neutron, which is almost twice that of a commercial
6
Li-glass (GS20) scintillator (7000 photons/thermal neutron). Effective neutron-gamma pulse discrimination was achieved using a network dynamics digital filter, effectively separating thermal neutron events from gamma events.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
YiRong Yao,Bing Xing,Jianbing Chen,YanLun Ren,YuJia Ma,Ying Zhang,Li Zhang
This study proposes an advanced method to tackle CO 2 emissions by enhancing solid acid catalysts, aiming to reduce the high energy consumption and low economic efficiency typically associated with chemical absorption processes. The research involves modifying commercial HZSM-5 zeolites through Cu ion exchange, with the optimal performance observed at a Cu ion content of 2.86 % and a Cu salt concentration of 0.2 M. This modification significantly minimizes the loss of copper ions—a common issue in the impregnation method—resulting in a 76.62 % reduction in the loss of active components. To further improve CO 2 gas-liquid mass transfer, mesoporous MCM-41 zeolites were introduced. Experimental results demonstrate that, at a regeneration temperature of 86°C and a mass ratio of 2:1 for HZSM-5 to MCM-41, the combined catalyst achieves a 61.28 % reduction in relative heat duty compared to the blank sample. Moreover, the energy consumption is 12.33 % and 16.45 % lower than that of HZSM-5 and MCM-41 used individually. Characterization analysis reveals that, under comparable acidic active site densities, catalysts with superior physical pore structures exhibit enhanced catalytic performance. The introduction of mesoporous structures notably improves the bidirectional mass transfer efficiency between carbamate macromolecules and CO 2 molecules. This work successfully demonstrates the synergistic effect of combining Cu ion-modified HZSM-5 zeolites with mesoporous MCM-41, leveraging the abundant active sites of HZSM-5 while harnessing the enhanced mass transfer properties of MCM-41.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Ganghua Zhou,Yun Chen,Gaoran Chen,Hangmin Xu,Weiqin Yin,Bin Wang,Xingwang Zhu,Xin Ning,Paul K. Chu,Xiaozhi Wang,Hui Xu
Metal-organic frameworks (MOFs) with abundant pores are excellent adsorbents for metal ions. However, the subsequent treatment of used MOFs and their reutilization still lack promising solutions. Herein, the surface-restructured Mn-doped Cu 2 O (RM-Cu 2 O) catalyst containing asymmetric Mn−Cu sites is prepared by glucose reduction using the spent Cu-based MOF (HKUST-1) as the precursor. The RM-Cu 2 O catalyst shows good potential in tunable photocatalytic syngas (CO and H 2 ) production in a pure water system. The syngas ratios can be tuned from ∼1:2 to ∼1:1 by increasing CO production. DFT calculations and photoelectrochemical tests confirm that the asymmetric Mn−Cu sites on the RM-Cu 2 O catalyst accelerate the photogenerated charge transport and optimize CO 2 adsorption and activation. In situ irradiation X-ray photoelectron spectroscopy is conducted to investigate the dynamic charge transport and reactions on the RM-Cu 2 O catalyst. Based on in situ Fourier transform infrared spectroscopy and simulations, the mechanism of photocatalytic syngas production is elucidated. This work provides a promising solution for the resource utilization of the spent MOFs-based adsorbents and photocatalytic energy development.
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DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 26
·10919-10927
·
IF 3.5
Xuanzhao Lu,Baozhen Yuan,Yi Liu,Li-Xia Liu,Jun-Jie Zhu
Electrochemical reduction of carbon dioxide (CO2) or carbon monoxide (CO) to valuable multi-carbon (C2+) products like acetate is a promising approach for a sustainable energy economy. However, it is still challenging to achieve high activity and selectivity for acetate production, especially in neutral electrolytes. Herein, a bioinspired hemin/Cu hybrid catalyst was developed to enhance the surface *CO coverage for highly efficient electroreduction of CO to acetate fuels. The hemin/Cu electrocatalyst exhibits a remarkable faradaic efficiency of 45.2% for CO-to-acetate electroreduction and a high acetate partial current density of 152.3 mA cm−2. Furthermore, the developed hybrid catalyst can operate stably at 200 mA cm−2 for 14.6 hours, producing concentrated acetate aqueous solutions (0.235 M, 2.1 wt%). The results of in situ Raman spectroscopy and theoretical calculations proved that the Fe–N4 structure of hemin could enhance the CO adsorption and enrich the local concentration of CO, thereby improving C–C coupling for acetate production. In addition, compared to the unmodified Cu catalysts, the Cu catalysts functionalized with cobalt phthalocyanine with a Co–N4 structure also exhibit improved acetate performance, proving the universality of this bioinspired molecule-enhanced strategy. This work paves a new way to designing bioinspired electrolysis systems for producing specific C2+ products from CO2 or CO electroreduction.
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FOOD HYDROCOLLOIDS
·
2024
·
IF 11
Peini Li,Yiqing Deng,Wangcai Zou,Zhenqiao Ma,Xiandi Yang,Qiang Zhao
As living standards improve, the demand for food freshness has gradually increased. Multifunctional packaging materials that monitor food freshness in real-time, delay spoilage, and are environmentally friendly have emerged as ideal solutions. This study synthesized an ammonia-sensitive copper-based metal-organic framework (Cu-MOF) and incorporated it into a matrix composed of chitosan (CS) and gelatin (Gel). The resulting film exhibits ammonia-sensitive color-changing properties, antibacterial activity, and excellent biodegradability. The effects of Cu-MOF incorporation on the structural, physical, and functional properties of the CS/Gel films were systematically evaluated. Results demonstrated that the Cu-MOF was uniformly distributed within the CS/Gel matrix, significantly enhancing the mechanical properties (tensile strength increased by 68.49%), oxygen/water vapor barrier properties, and UV-blocking capability of the films. Notably, the CS/Gel@Cu-MOF films exhibited excellent antibacterial performance, with sterilization rates of 94.2% against Escherichia coli and 99.6% against Staphylococcus aureus . Additionally, the films showed good biocompatibility, biodegradability, and a sensitive color response to ammonia. The films were successfully used to monitor shrimp freshness through color change, transitioning from light green to brown as spoilage occurred. These findings indicate that CS/Gel@Cu-MOF films have significant potential for real-time visual freshness monitoring in food packaging, contributing to reduced food safety risks and waste.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Fu Li,Qian Huo,Xiaomei Zhou,Shasha Fang,Fei Han,Jingnan Yang,Qingxin Guan,Wei Li
Photothermal CO 2 into methanol is an effective approach to address energy and environmental challenges, but the low conversion and poor selectivity limit its large-scale application. Here, 0.5Cu@CeO 2 with atomically dispersed active sites and abundant Frustrated-Lewis-pairs (FLPs) was synthesized using coordination complex precipitation reaction. The substitution of Cu 2+ with Ce 3+ results in the formation of new FLPs, which promotes the upward shift of conduction band (CB) and enhances the reducing capability of catalyst. Moreover, the more sensitive and stronger capability of photogenerated carriers also endows 0.5Cu@CeO 2 with stronger CO 2 reduction capability. The photothermal methanol yield of 0.5Cu@CeO 2 reached 1896.02 μmol·g cat –1 ·h –1 . The DFT results demonstrate the FLPs structure of 0.5Cu@CeO 2 promotes parallel adsorption of CO 2 and *CO species. Meanwhile, the presence of O v inhibits the dissociation of oxygen species, consequently boosting the methanol synthesis. The construction of FLPs structure introduces a novel method to enhance CO 2 conversion utilizing photothermal catalysis.
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