ACS Catalysis
·
2025
·
IF 13.1
Jia-qi Bai,Mei Ma,Huangfei Liu,Zhangkai Qian,Durui Liu,Yuncai Zhao,Yijing Gao,Jingshuai Chen,Mengdie Cai,Song Sun
The hydrogenation of nitriles is an environmentally friendly and atom-economical route to prepare high-value amines; however, it is still a challenge to control selectivity because of the occurrence of hydrogenation, self-coupling, and hydrogenolysis reactions during the hydrogenation process. It is highly desirable to develop efficient non-noble-metal catalysts for the hydrogenation of nitriles to secondary amines, although several noble metal catalysts have been reported. Herein, we successfully prepared a Cu–Ni/W20O58 catalyst and found that the Cu4.4–Ni0.6/W20O58 catalyst showed a 92.3% yield with initial TOFs of 270.0 h–1 at 373 K and 3 MPa H2 for the hydrogenation of benzonitrile (BN) to dibenzylamine (DBA), which was much superior to that of the monometallic Cu4.4/W20O58 and Ni0.6/W20O58 catalysts. Moreover, the Cu4.4–Ni0.6/W20O58 catalyst could be reused at least 4 times and was effective for the hydrogenation of various nitriles with superior selectivity to secondary amines. Furthermore, the reaction mechanism of BN hydrogenation for the Cu–Ni alloy of Cu4.4–Ni0.6/W20O58 was proposed on the basis of spectroscopic studies such as XRD, TPR, TEM, XAFS, and XPS, kinetic studies such as the effect of BN concentration and H2 pressure, the isotopic effect of hydrogen, and the effect of the reaction temperature and DFT calculations. The rate-determining step was the hydrogenation of benzylidenamine (BI) to the half-hydrogenated intermediate by one H atom over the Cu4.4–Ni0.6/W20O58 catalyst. The Ni–W20O58 interface was responsible for the adsorption and activation of BN, and the electron-rich Cu acted as the site for H2 dissociation; the synergistic effect of Cu and Ni led to the superior catalytic performance of the Cu4.4–Ni0.6/W20O58 catalyst.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhuo Ma,Yihui Li,Zheng Li,Ziyin Liu,Xuepeng Wang,Yuan Tan,Xingkun Chen,Wei Lu,Yunjie Ding
Increasing dimethyl oxalate (DMO) hydrogenation activity remains a challenge. A Cu catalyst was designed by creating Cu nanoparticles (NPs) over SiO 2 layer formed on the CeO 2 particles (SiO 2 @CeO 2 ) using the ammonia evaporation method followed by the calcination and reduction step. The optimized 30Cu/SiO 2 @5CeO 2 catalyst shows good performance in the micro-packed bed reactor (100 % DMO conversion, 95.9 % ethylene glycol (EG) selectivity, 200 h stability) under the condition of the ratio of H 2 to DMO (H 2 /DMO) = 30, 190 °C and 2 MPa in the run, and CeO 2 was proved to be effective in the DMO hydrogenation process. The exposed CeO 2 on the surface of catalyst was found to facilitate the formation of Cu + by its interaction between adjacent Cu nanoparticles, resulting in the faster adsorption and dissociation of C=O bond on the catalyst surface, according to the characterization results obtained by the XRD, XPS and in situ FT-IR, etc.
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Nano Research
·
2024
·
IF 9.5
Shen Huidong,Yang Chunming,Hong Song,Hao Leiduan,Xu Liang,Robertson Alex W.,Sun Zhenyu
Semiconductor-based photocatalysis by utilizing solar energy for sustainable organic pollutant elimination has been a promising tactic to alleviate environmental issues. Nevertheless, the development of robust and efficient photocatalysts to degrade organic pollutants still faces major challenges because of insufficient charge separation. Here we design and fabricate a heterojunction consisting of copper, carbon-modified TiO 2 , and sulfur-doped g-C 3 N 4 nanosheets (i.e., S-C 3 N 4 /Cu/C-TiO 2 ). The heterostructure affords a remarkable synergistic photocatalysis for tetracycline hydrochloride degradation, achieving an 82.6% removal efficiency within 30 min under visible light irradiation, about 15.4 and 7.3 times higher than that of S-C 3 N 4 and C-TiO 2 , respectively. The superior performance is attributed to the synergy between Cu doping and the Z-scheme heterojunction, which not only enhances the interfacial electric field effect, facilitating charge separation, but also boosts the redox capability. The charge carrier transfer between Cu/C-TiO 2 and S-C 3 N 4 follows a Z-scheme, as verified by trapping experiments, electron spin-resonance spectroscopy, and density functional theory calculations. Furthermore, the tetracycline hydrochloride degradation pathways are enunciated by liquid chromatograph mass spectrometry analysis. This work provides an effective approach for constructing high-performance photocatalysts that have potential in environmental remediation.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Zhengyan Hao,Yong Xu,Xijia Yang,Xuesong Li,Yang Gao,Liying Wang,Wei Lü
Zinc-ion hybrid supercapacitors (ZIHSCs) are emerging as a promising energy storage device, combining the benefits of traditional batteries and capacitors, including high energy density, incredible power density, a wide voltage window, and excellent capacity retention. In this study, a Cu²⁺ and Zn²⁺ co-doped needle-like tunnel-structured α-MnO₂ material is proposed as the cathode (Cu-Zn-MnO₂@CC), which is grown on an acid-treated flexible carbon cloth substrate using a simple hydrothermal synthesis method. Along with an anode made of super-mesoporous activated carbon derived from waste rice husks (ACrh@CC). The synergistic effect of the co-doping stabilizes the nanowire tunnel structure and provides more active sites. As a result, the Cu-Zn-MnO₂@CC//2 M ZnSO₄//ACrh@CC ZIHSC achieves an ultrahigh specific capacitance of 1241.85 mF cm⁻² at 1 mA cm⁻², representing an improvement of more than 50 % in performance compared to with conventional MnO₂@CC ZIHSC. And a maximum areal energy density of 689.9 μWh cm⁻² at a power density of 1 mW cm⁻². After 20,000 cycles, it retains 86.35 % of its initial capacitance. Furthermore, the assembled flexible device achieves a specific capacitance of 1070.21 mF cm⁻² at 1 mA cm⁻². This device can provide long-term power for electronic devices such as digital watches and timers. The study offers crucial understanding regarding structure of ZIHSC electrode materials and opens up possibilities for their potential applications.
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Coatings
·
2024
·Vol. 14
·期 4
·453
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IF 2.9
Ningning Xing,Lilin Yang,Li Wang,Yanxiang Lu,Hongkun Zhang,Xijun Sun,Min Zhao,Wenjie Tan,Jie Yang
The reliable detection of environmental contaminants can correctly forecast the degree of environmental pollution that has occurred, which contributes to improving the environmental purification rate and maintaining the ecological balance. Herein, a novel hierarchical biomimetic catalysis MnO2@CuAl-CLDHs was designed and synthesized using a facile method, which exhibited significantly enhanced peroxidase-like activity due to the unique composition and hierarchical mesoporous structure. Under optimized operational conditions, a visible colorimetric array based on the superior nanozyme activity of MnO2@CuAl-CLDHs was developed for the quantitative determination of hydroquinone with a wide linear detection range (1–100 μM) and a low detection limit (0.183 μM). Simultaneously, our presented strategy could analyze hydroquinone in real water samples with high accuracy. Therefore, the bimetallic co-catalyzed nanozymes are expected to be the perfect replacement for natural enzymes to develop convenient and efficient sensors.
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INDUSTRIAL CROPS AND PRODUCTS
·
2025
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IF 6.2
Yajun Liu,Yongzhi Xiong,Chenxin Jin,Changzhou Chen,Liangliang Zhang,Jianchun Jiang,Jingcong Xie
Herein, a novel hydrothermal synthesis strategy is proposed for the preparation of novel Cu-Ce MOF heterojunction nano catalysts (CuCeO X /C) for 5-hydroxymethylfurfural (HMF) electrooxidation reaction in this paper. CuCeO X /C exhibits superior catalytic performance, with the current density of CuCeO X /C reaching 100 mA cm −2 at a low potential of 1.408 V vs. RHE, and doubling to 280 mA cm −2 at a lower potential of 1.5 V vs. RHE. Under these conditions, the conversion of HMF reaches 100 %, with a selectivity of over 99.11 % for 2,5-furan dicarboxylic acid (FDCA) and a Faradaic efficiency of 97.76 %. Theoretical calculations and In-situ-EIS have demonstrated that Ce-based Cu-MOF heterojunction nanocatalysts enhance the adsorption energy of the CuCeO X /C catalysts on HMF substrates while also decreasing reaction energy barrier of HMFOR. Based on our work, the employment of CeCu/MOF heterojunction electrocatalysts for efficient electro-oxidation of HMF to FDCA paves a green and sustainable way for advancing sustainable chemical processes and biomass valorization.
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ACS Catalysis
·
2025
·
IF 13.1
Shiyan Li,Xu Liu,Jun Ma,Feifei Xu,Yuan Lyu,Siglinda Perathoner,Gabriele Centi,Yuefeng Liu
The high-temperature reverse water–gas shift (RWGS) is an industrially relevant reaction. Cu-based catalysts easily sinter and deactivate under these conditions. We demonstrate that it is possible to obtain high-performance and stable catalysts by modifying the mechanism of action. Cu/CeOx-MgO (denoted as Cu/CexMgy) catalysts were developed in which Cu nanoparticles mostly generate spillover H that migrates to support sites where CO2 is selectively reduced, with the rate controlled by the oxide–oxide CeOx-MgO interface. An optimal Cu/Ce0.05Mg0.95 catalyst (in terms of performance at the lowest possible Ce amount) exhibits a near-equilibrium CO2 conversion with a reaction rate of 516.0 μmol·gcat–1·s–1, near-total selectivity to CO at 600 °C, and a high space-velocity of 300,000 mL·gcat–1·h–1. These are among the top performances in the RWGS reaction. Extensive characterization data have proven that the surface-abundant Ce-[Ov]-Mg sites play a critical role in CO2 adsorption/activation as well as the carrier for the spillover of hydrogen species. The mechanism is substantially different from those indicated for Cu-based catalysts for CO2 hydrogenation. By decoupling H and CO2 activation sites and realizing efficient surface mobility of H-spillover species via an enhanced oxide–oxide interface, it is possible to maintain the overall stability and activity of the catalyst when the Cu nanoparticles sinter at a high temperature (i.e., ≥600 °C).
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Yi Gao,Tingting Chu,Chengyu Zhou,Wensheng Huang,Yin Zheng
In this paper, iron–copper bimetallic nanosheet materials (FeCu/CNS) were prepared using hydrothermal and pyrolysis methods to develop a dual-mode electrochemical and colorimetric sensing platform for detecting acetaminophen (ACM). The glassy carbon electrode (GCE) was modified with FeCu/CNS to enhance its electrocatalytic activity and develop an electrochemical sensor for detecting ACM. The linear range of the sensor was 0.01–7 × 10–6 mol/L, and the detection limit (LOD) was 2.5 × 10–8 mol/L. In addition, FeCu/CNS possesses an efficient peroxidase-like activity that converts colorless 3,3′,5,5′-tetramethylbenzidine (TMB) into a blue oxidized state product (oxTMB) in the presence of H2O2, which exhibits a characteristic absorption peak around 652 nm. However, ACM has reducing properties and can reduce oxTMB to TMB, thereby reducing the intensity of the characteristic absorption peak of oxTMB. Based on this principle, a colorimetric sensor was constructed for the detection of ACM, which had a linear range of 0.5–1625 × 10–6 mol/L and an LOD of 2.63 × 10–6 mol/L. Compared with other single methods, the method exhibited a wider linear range and lower detection limit, confirming the complementary and superior nature of the dual-mode sensor designed in this paper for ACM detection. Meanwhile, the detection of ACM in human serum was also carried out with satisfactory results.
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SCRIPTA MATERIALIA
·
2024
·
IF 5.3
Mengyun Jia,Dingliang Liang,Qing Du,Hui Wang,Yuan Wu,Suihe Jiang,Xiaobin Zhang,Haihui Ruan,Xiongjun Liu,Zhaoping Lu
Magnetothermal therapy (MT) is a noninvasive cancer treatment that has shown great promise in recent years. However, the low magnetothermal efficiency of the existing magnetic nanoparticles used in MT has been an obstacle to their widespread applications. In this work, we report a new class of Fe-Co-Ni-Cu high-entropy magnetic nanoparticles (HEMNPs) with exceptional magnetothermal properties synthesized by a thermal decomposition method. The fabricated HEMNPs, having an average diameter of 60–70 nm, exhibited a saturation magnetization of 42.4 emu/g and coercivity of 129.5 Oe. The hyperthermia measurement reveals that the HEMNPs have a maximum specific loss power of 202 W/g at the concentration of 2 mg/ml under an alternating magnetic field with an intensity of 46 Oe and a frequency of 266 kHz, demonstrating the great potential for MT applications. Our results demonstrate that the high-entropy concept can be extended to develop high-performance magnetic nanoparticles for MT applications.
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Surfaces and Interfaces
·
2025
·
IF 6.3
Chenghao Zhang,Changlong Tan,Yang Liu,Chun Li,Xiaoqing Si,Zongjing He,HaiFeng Zhang,Jian Cao
The fabrication of surfaces with varying wettability is crucial for developing Janus materials. In this study, a Janus Cu/Ti mesh with asymmetric wetting surfaces is fabricated using diffusion bonding. The Ti and Cu meshes are bonded through vacuum hot-pressing, forming a two-layer compositing, and the CuTi intermetallic compound is found at the interface. High-density TiO 2 nanostructures are synthesized on the Ti wire via hydrothermal treatment in NaOH. Subsequent immersion in a stearic acid solution, renders the Cu mesh hydrophobic, while the Ti mesh retains its hydrophilic properties, resulting in a Janus Cu/Ti mesh with asymmetric hydrophobic/superhydrophobic behavior. The unidirectional transport properties of this Janus mesh, including water penetration and bubble/oil manipulation, are systematically studied. Additionally, a superhydrophobic/hydrophilic Janus mesh is achieved by synthesizing CuO nanosheets on Cu mesh and applying surface modifications. This approach broadens the technological framework for fabricating Janus materials and enhances the potential applications of diffusion bonding, highlighting its versatile prospects.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Jia-Xu Shuang,Jie Sheng,Yunzhong Wu,Manyu Liu,Changsheng Xing,Rui Liu,Tong Zhang,Bin Liu,Yekang Guan,Lidong Wang,Weidong Fei
Graphene/copper composites demonstrate outstanding mechanical and electrical properties, making them suitable for a wide range of applications. Among the various methods for preparing graphene/copper composites, the in-situ synthesis approach has gained significant attention due to its simplicity and potential for commercial scalability. In this study, we report a mechanochemical method that utilizes terphenyl as a carbon source for the in-situ preparation of Gr/Cu composites. In this approach, mechanical force is utilized to induce polymerization of terphenyl, as opposed to thermal catalysis. Compared to pure copper, the yield strength of the composite with 0.1 wt% carbon addition increased by 13.7%, and its conductivity improved by 3.8%IACS. The composite also exhibited a higher strengthening efficiency of 86.7%. A harmonic structure within the composite was observed, which contributes to increased strength while maintaining a certain degree of plasticity. The structural evolution of graphene during the mechanochemical process was analyzed, and a hypothesis was proposed to explain the structure changes during polymerization. This study presents a novel method and valuable insights for the preparation of Gr/Cu composites through mechanochemical processes.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Lixin Song,Guobin Liu,Zhenping Qu
CO 2 hydrogenation to methanol and/or dimethyl ether (DME) holds promise for mitigating greenhouse gas effects and addressing energy scarcity. However, the relationship between product selectivity and the collective nature of the catalysts remains ambiguous due to the intricate reaction network. Here, a series of Cu/Zn x Al y O z catalysts with different surface properties have been engineered by manipulating the Zn/Al ratio to achieve product controllability for CO 2 hydrogenation. The results unveil the pivotal role of the H 2 dissociation capability in governing CO 2 conversion, which is regulated by the concentration of Cu 0 species. Furthermore, the number of surface hydroxyl groups, the proportion of moderately strong basic sites and moderately strong acidic sites show desirable linear correlations with the selectivity of CO, CH 3 OH, and DME, respectively. Importantly, the ZnAl 2 O 4 -Al 2 O 3 or Cu-ZnAl 2 O 4 -Al 2 O 3 interface notably enhances moderately strong acidic sites, aiding methanol dehydration to DME. This work offers a comprehensive guide to the rational design of catalysts for oriented product synthesis from CO 2 hydrogenation.
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