Journal of Environmental Sciences
·
2025
·
IF 6.3
Yansen Qu,Xin Li,Yingjie Xia,Haosheng Lan,Le Ding,Jing Zhong,Xinghua Chang
Accelerated industrialization combined with over-applied nitrogen fertilizers results in serious nitrate pollution in surface and ground water, disrupting the balance of the global nitrogen cycle. Electrochemical nitrate reduction (eNO 3 RR) emerges as an attractive strategy to simultaneously enable nitrate removal and decentralized ammonia fabrication, restoring the globally perturbed nitrogen cycle. However, complex deoxygenation-hydrogenation processes and sluggish proton-electron transfer kinetics significantly hinder practical application of eNO 3 RR. In this study, we developed carbon-coated Cu-Ni bimetallic catalysts derived from metal-organic frameworks (MOFs) to facilitate eNO 3 RR. The unique structural features of catalyst promote enhanced synergy between Cu and Ni, effectively addressing critical challenges in nitrate reduction. Comprehensive structural and electrochemical analysis demonstrate that electrochemical nitrate-to-nitrite conversion mainly takes place on active Cu sites, the introduction of Ni could efficiently accelerate the generation of aquatic active hydrogen, promoting the hydrogenation of oxynitrides during eNO 3 RR. In addition, Ni introduction could push up the d-band center of the catalyst, thus enhancing the adsorption and activation of nitrate and the corresponding intermediates. Detailed reaction pathways for nitrate-to-ammonia conversion are illuminated by rotating disk electrode (RDE), in-situ Fourier-transform infrared spectroscopy, in-situ Raman spectrum and electrochemical impedance spectroscopy (EIS). Benefiting from the synergistic effect of Cu and Ni, optimum catalyst exhibited excellent nitrate reduction performance. This work provides a new idea for elucidating the underlying eNO 3 RR reaction mechanisms and contributes a promising strategy for designing efficient bimetallic electrocatalysts.
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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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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
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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 COLLOID AND INTERFACE SCIENCE
·
2024
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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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Nanomaterials
·
2024
·Vol. 14
·期 24
·2000
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IF 4.4
Zhipeng Yu,Pengxu Yan,Yilei Sheng,Chengwei Zhang,Zhun Qiao,Qikui Fan,Chuncai Kong,Zhimao Yang
Copper-based materials, renowned for their redox versatility and conductivity, have extensive applications in electrochemical sensing. Herein, we construct stable Cu+/Cu2+interfaces within dual-valence copper nanostructures to achieve enhanced sensitivity in glucose sensing. By employing a hydrolysis method to tune Cu2+/Cu+ratios precisely, we achieved an optimal electrochemical interface with heightened stability and reactivity. The Cu+/Cu2+interface-based flexible electrode demonstrated excellent glucose sensitivity (332.4 µA mmol/L−1cm−2at +0.65 V), wide linear range (up to 10 mmol), a low detection limit of 1.02 nmol/L, and strong selectivity, including detection in human sweat, making this study significant for advanced electrochemical sensors.
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Inorganic Chemistry Frontiers
·
2024
·
IF 6.1
Yifei Li,Senyao Meng,Ping Wang,Miao He,Jiasai Yao,Cheng Yang,Fangzhou Mo,Jiang Li,Zhenxing Li
The crystal facet of CeO2 is crucial in governing the catalytic performance of CeO2. However, studies on the relationship between the photocatalytic oxidation performance of CeO2 and its crystal facets are scarce. Herein, we synthesized a series of CeO2. Through loading Cu single atoms (Cu/CeO2), the facet effects of crystal facets on photocatalytic selective oxidation were systematically studied by employing the selective oxidation of 5-hydroxymethylfurfural to 2,5-diformylfuran as a model. Because the (110) facet's superior electron transfer efficiency is feasible for absorbing 5-hydroxymethylfurfural, eliminating α-H, and desorbing 2,5-diformylfuran, the selectivity of Cu/CeO2-nanorods (Cu/CeO2-R) with the (110) facet (93.34%) is much higher than that of Cu/CeO2-nanocubes (Cu/CeO2-C) with the (100) facet (32.22%) and Cu/CeO2-nanooctahedra (Cu/CeO2-O) with the (111) facet (15.20%). DFT calculation shows that Cu 3d exhibits orbital hybridization with Ce 5d and 4f, which provides a favorable pathway for electron transfer. This work delves into the facet-performance relationship during the photocatalytic process.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jiankang Wang,Shuhong Liu,Ping Song,Xiao Zhang,Ying Song,Wanqian Guo,Zhongping Yao
Nanoparticle aggregation and metal ion leaching contribute to the poor cycling stability of nanostructured zero valent copper (ZVC) catalyst for molecular oxygen activation, greatly hindering its industrial application in wastewater treatment. Herein, N doped carbon coated Cu 0 (Cu@CN) catalysts were prepared by using polyvinylpyrrolidone (PVP) modified Cu-MOF as precursor through high-temperature pyrolysis method. The phase structure, surface morphology and microstructure information of as-synthesized catalyst were systematically characterized by XRD, Raman, SEM, XPS and TEM. Norfloxacin (NOR) degradation in Cu@CN/air system showed Cu@CN3-600, prepared by using 0.3 g PVP as N source and pyrolysis temperature of 600 ℃, exhibited excellent catalytic activity and stability as well as universality in treating various organic wastewaters. The removal rate of NOR after 60 min was 96.05 % and meantime total organic carbon (TOC) decreased by 49.80 % under pH 4.0 and 1.2 g/L catalyst. After three cycles, it still maintained 81.53 % removal rate, owing to the protection effect of N doped carbon on active Cu component against its leaching during degradation. The reaction mechanism of Cu@CN3-600 activating O 2 for NOR degradation was deciphered by reactive oxygen species scavenging experiment, electron paramagnetic resonance (EPR) and density functional theory (DFT) calculation. Finally, four possible degradation pathways were proposed by identifying 16 intermediates through liquid chromatography-mass spectrometry (LC-MS) technology. This work can provide a guidance for designing highly efficient Cu-based molecular oxygen activation catalyst for wastewater abatement.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Ze Li,Wen-Jie Li,Jun Guo,Zi-Yuan Wang,Xing Yang,Yu-Ke Zhu,Tian-En Shi,Yi-Xin Zhang,Jing Feng,Zhen-Hua Ge
SnSe materials have attracted extensive attention in thermoelectrics due to their low thermal conductivity. Nevertheless, the thermoelectric properties of n-type polycrystalline SnSe are still low, and metallic Sn distributed in the SnSe1–x materials would affect the repeatability of thermoelectric performance. Herein, the thermoelectric properties of n-type polycrystalline SnSe0.95-based composites are highly enhanced by heterogeneous Cu doping. The carrier concentration of the SnSe0.95 material was optimized by SnCl2 doping. The strategy of heterogeneous Cu doping is employed in further improving the thermoelectric performance of the SnCl2-doped SnSe0.95 materials. In addition, partial Cu+ doping tunes the electron concentration to enhance the Seebeck coefficient. Moreover, metallic Sn distributed along the grain boundaries can be stabilized by forming Cu6Sn5 alloys, which improve the thermal stability of bulk composites. Excessive Cu particles and SnCl2 precipitates strengthen phonon scattering for lowering the lattice thermal conductivity. Ultimately, a peak ZT of 1.55 is yielded at 773 K in the SnSe0.95–1 wt % SnCl2–1 wt % Cu bulk composite, whose mechanical hardness is also increased. Hence, these results promote a feasible approach to simultaneously enhance the thermoelectric and mechanical properties of n-type SnSe-based composites, which might be worth exploring in other thermoelectric materials.
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CHEMICAL PHYSICS LETTERS
·
2024
·
IF 2.8
Ye Liu,Lei Zhang,Yubo Kuang,Xiaoqian Xiang,Haohan Tao,Guangran Di,Xiaojing Yin,Meicheng Li,Xiao-Jun Lv
The photocatalytic CO 2 reduction has the problems of low selectivity of single product. Here, the preparation of Cu modified tubular C 3 N 4 (CTN) was studied. The increase of the active site inhibits the recombination of electrons (e-) and holes (h + ) and improves the selectivity of CO 2 reduction products. Finally, the CO and CH 4 yields of 1.5 % CTN photocatalyst are 11.55 μmol·g −1 and 4.72 μmol·g −1 , respectively, which are 5 times higher than that of tubular C 3 N 4 photocatalyst. The selectivity of 2 % CTN to CH 4 is up to 68 %, indicating that the prepared CTN photocatalyst has high CO 2 reduction activity and CH 4 selectivity.
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ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Lan-Ying Liu,Min-Hua Cui,John Justo Ambuchi,Shi-Ming Niu,Xin-Hui Li,Wo-Long Wang,He Liu,Guo-Shuai Liu,Ai-Jie Wang
Electrocatalytic hydrodechlorination (EHDC) is a promising approach to safely remove halogenated emerging contaminants (HECs) pollutants. However, sluggish production dynamics of adsorbed atomic H (H* ads ) limit the applicability of this green process. In this study, bimetallic Pd–Cu@MXene catalysts were synthesized to achieve highly efficient removal of HECs. The alloy electrode (Pd–Cu@MX/CC) exhibited better EHDC performance in comparison to Pd@MX/CC electrode, resulting in diclofenac degradation efficiency of 93.3 ± 0.1%. The characterization analysis revealed that the Pd 0 /Pd II ratio decreased by forming bimetallic Pd–Cu alloy. Density functional theory calculations further demonstrated the electronic configuration modulation of the Pd–Cu@MXene catalysts, optimizing binging energies for H* and thereby facilitating H* ads production and tuning the reduction capability of H* ads . Noteably, the amounts and reduction potential of H* ads for Pd–Cu@MXene catalysts were 1.5 times higher and 0.37 eV lower than those observed for the mono Pd electrode. Hence, the introduction of Cu into the Pd catalyst optimized the dynamics of H* ads production, thereby conferring significant advantages to EHDC reactions. This augmentation was underscored by the successful application of the alloy catalysts supported by MXene in EHDC experiments involving other HECs, which represented a new paradigm for EHDC for efficient recalcitrant pollutant removal by H* ads .
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LANGMUIR
·
2025
·
IF 3.9
Lihuan Wang,Yanbing Dong,Liting Yuan,Xinxin Li,Yuan Li,Bingyan Li,Zijin Liu,Jinpeng Mo,Dongliang Dai,Xi Yu,Hui Yu
Inorganic nanofibers have emerged as a promising frontier in biomedical research thanks to their unique nanomorphology and bioactivity. Furthermore, the ions released from these inorganic biomaterials play a crucial role in determining cell identity and driving tissue-specific functions. Notably, Cu and Mn, which are essential trace elements in the human body, play significant roles in promoting bone health and participating in metabolic processes. Therefore, in this study, a series of Cu/Mn-doped SiO2–CaO composite nanofibers (CNFs) prepared by sol–gel electrospinning were obtained, and their morphology, flexibility, mineralization property, photothermal property, and antibacterial activity were studied. Experimental research has shown that the 2.5Cu and 2.5Mn CNFs calcined at 800 °C have the best flexibility, and as the Cu/Mn content or calcination temperature increases, the flexibility of CNFs decreases. In addition, 10Cu and 10Mn CNFs calcined at 800 °C have the best photothermal property, reaching temperatures of 65 and 62 °C under near-infrared irradiation (NIR) of 2 W cm–2 in the wet state, respectively, and the increase in calcination temperature results in decreased photothermal temperatures. The bacterial inhibition rates of CNFs (5Cu and 5Mn) with and without NIR are over 89 and 68%, respectively. The mineralization experiment also proved that Cu/Mn-doped CNFs have excellent mineralization activity. Therefore, these Cu/Mn-doped CNFs with excellent flexibility, photothermal property, mineralization activity, and antibacterial ability show great application potential in the treatment of tumors and bone defect-related diseases.
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