Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
·
IF 14.7
Liu Shikai,Li Yuheng,Wang Di,Xi Shibo,Xu Haoming,Wang Yulin,Li Xinzhe,Zang Wenjie,Liu Weidong,Su Mengyao,Yan Katherine,Nielander Adam C.,Wong Andrew B.,Lu Jiong,Jaramillo Thomas F.,Wang Lei,Canepa Pieremanuele,He Qian
The reconstruction of Cu catalysts during electrochemical reduction of CO 2 is a widely known but poorly understood phenomenon. Herein, we examine the structural evolution of Cu nanocubes under CO 2 reduction reaction and its relevant reaction conditions using identical location transmission electron microscopy, cyclic voltammetry, in situ X-ray absorption fine structure spectroscopy and ab initio molecular dynamics simulation. Our results suggest that Cu catalysts reconstruct via a hitherto unexplored yet critical pathway - alkali cation-induced cathodic corrosion, when the electrode potential is more negative than an onset value ( e.g ., −0.4 V RHE when using 0.1 M KHCO 3 ). Having alkali cations in the electrolyte is critical for such a process. Consequently, Cu catalysts will inevitably undergo surface reconstructions during a typical process of CO 2 reduction reaction, resulting in dynamic catalyst morphologies. While having these reconstructions does not necessarily preclude stable electrocatalytic reactions, they will indeed prohibit long-term selectivity and activity enhancement by controlling the morphology of Cu pre-catalysts. Alternatively, by operating Cu catalysts at less negative potentials in the CO electrochemical reduction, we show that Cu nanocubes can provide a much more stable selectivity advantage over spherical Cu nanoparticles.
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PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Wei Zhou,Mazhar Ahmed Memon,Mengmeng Niu,Xinqiang Fan,Yanan Jiang,Xian Zhang,Yuan Liu
Copper (Cu) based catalysts are frequently used in CO 2 hydrogenation, particularly in reverse water-gas shift (rWGS) and CO 2 -to-methanol reaction. Cu 0 and Cu + are the key species affecting the catalyst performance and product distribution . Therefore, constructing and adjusting Cu 0 /Cu + active pairs is significant for the catalyst design . In this study, Cu 0 /Cu + active pairs are obtained by utilizing the properties of perovskite-type oxides (PTOs). A series of CaTi 1-x Cu x O 3 and Ca 0.8 La 0.2 Ti 1-x Cu x O 3 (x = 0.05, 0.10, 0.15, 0.30, 0.40 and 0.50) were synthesized via citric acid complexing method and part of the Cu species entered the PTOs lattice. After reduction, large Cu particles and highly-dispersed Cu clusters were obtained simultaneously. The dispersed Cu clusters have more interfaces with the PTOs and provide abundant Cu + while large Cu particles tend to aggregate and supply mainly Cu 0 . Cu 0 activates H 2 and CO 2 and plays a vital role in the rWGS reaction . Cu + is the active site for methanol synthesis and it can strongly absorb CO. The ratio of Cu 0 /Cu + varies with different Cu content and doping La can also adjust the chemical state of surface Cu. The performance test demonstrates that both excessively high and low Cu 0 /Cu + ratios are beneficial for CO generation, while a moderate ratio is suitable for methanol synthesis . These insights provide a method for regulating the chemical state of surface metal species and help the catalyst design for CO 2 hydrogenation.
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FIBERS AND POLYMERS
·
2017
·Vol. 18
·期 7
·1250-1254
·
IF 1.113
Chen Yingbo,Liu Huiqiang,Hu Xiaoyu,Cheng Bowen,Liu Dongqing,Zhang Yufeng,Nair Sankar
Membranes with high water permeation capability as well as high rejection to dye molecules are very important for dye separation. In this study, a metal organic framework structure (Cu-BTC) was fabricated in situ on a poly(vinyl difluoride) hollow fiber support for nanofiltration of dye solution. In order to protect the Cu-BTC layer, the surface was coated by crosslinking polyvinyl alcohol. The composite membranes showed no rejection to divalent salts and high rejection to Congo Red dye. It was noticed that several Cu-BTC layers could enhance dye rejection of the composite membranes. This novel composite membrane showed promising applications in the separation of dye molecules from aqueous solutions containing dissolved salts.
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VACUUM
·
2021
·
IF 3.627
Ruifang Chen,Bixia Wen,Hong Li,Mingwu Xiang,Changwei Su,Junming Guo,Wei Bai,Zhaoyao Sa
A series of LiMn 2-x Cu x O 4 (0 ≤ x ≤ 0.1) cathode materials were synthesized via a rapid microwave-induced solution flameless combustion technique, and the structure, morphology and electrochemical performances of the LiMn 2-x Cu x O 4 samples were investigated in detail. All the as-prepared samples are the single crystal materials with a high crystallinity and correspond to the well-defined spinel structure. The spinel structure stability is effectively improved by the appropriate Cu-doping that is conducive to increasing the average valence of Mn and reducing lattice parameter . Consequently, the optimized LiMn 1.925 Cu 0.075 O 4 sample delivers a first discharge specific capacity of 108.5 mAh g −1 at 1 C and achieves the long-term charge/discharge cycle of 1000 cycles. At high current rate of 5 C and 10 C after 1000 cycles, the capacity retention of over 61% can be maintained. Even at the elevated temperature of 55 °C, the high initial capacity of 111.4 mAh g −1 and capacity retention of 63.91% are also delivered after 100 cycles at 1 C. This is ascribed to the favorable Li + diffusion kinetics, low charge transfer resistance and apparent activation energy .
研究领域:
材料科学
·
能源存储技术
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高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-9
·
IF 16.6
Feng Sihua,Duan Hengli,Tan Hao,Hu Fengchun,Liu Chaocheng,Wang Yao,Li Zhi,Cai Liang,Cao Yuyang,Wang Chao,Qi Zeming,Song Li,Liu Xuguang,Sun Zhihu,Yan Wensheng
The development of two-dimensional (2D) magnetic semiconductors with room-temperature ferromagnetism is a significant challenge in materials science and is important for the development of next-generation spintronic devices. Herein, we demonstrate that a 2D semiconducting antiferromagnetic Cu-MOF can be endowed with intrinsic room-temperature ferromagnetic coupling using a ligand cleavage strategy to regulate the inner magnetic interaction within the Cu dimers. Using the element-selective X-ray magnetic circular dichroism (XMCD) technique, we provide unambiguous evidence for intrinsic ferromagnetism. Exhaustive structural characterizations confirm that the change of magnetic coupling is caused by the increased distance between Cu atoms within a Cu dimer. Theoretical calculations reveal that the ferromagnetic coupling is enhanced with the increased Cu-Cu distance, which depresses the hybridization between 3 d orbitals of nearest Cu atoms. Our work provides an effective avenue to design and fabricate MOF-based semiconducting room-temperature ferromagnetic materials and promotes their practical applications in next-generation spintronic devices.
研究领域:
材料科学
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凝聚态物理
·
自旋电子学
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高影响因子
APPLIED COMPOSITE MATERIALS
·
2022
·Vol. 29
·期 6
·2147-2163
·
IF 2.368
Wang Pei,Guo Yonggang,Du Sanming,Jia Yunchao,Zhang Hongbo,Yin Jian
Taking the advantages of porous ceramic (C/C-SiC composite) and transpiration cooling (Copper alloy), C/C-SiC-Cu composite was fabricated to attain a novel anti-ablation material for high temperature structure application of aerospace systems, via chemical vapor deposition and infiltration technologies. The effects of SiC content on microstructure, thermal conductivity, mechanical and ablation properties of C/C-SiC-Cu composite were investigated. As the SiC content increases from 0 vol% to 25.12 vol%, thermal conductivity, flexural strength and ablation resistance are improved by 84.99%, 78.76% and 53.68%, respectively. Thermal conductivity and thermal diffusivity exhibit proportional linear correlation with SiC content. The high SiC content could shorten the yield stage and increase the breaking strength during the flexural fracture process. When the SiC content is 25.12 vol%, the formation continuous and compact anti-ablation (SiO 2 ) layer is formed by oxidizing and melting fluidity processes during oxyacetylene ablation test, and the protective layer covers the ablation surface and slows down the oxidative ablation, which combines with the transpiration cooling effect of copper alloy to further improve ablation resistance of C/C-SiC-Cu composite.
研究领域:
航空航天材料科学
·
高温结构材料
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Lanwei Li,Chengxiao Peng,Jing Chen,Zheng Ma,Yanqun Chen,Shuyao Li,Jianli Wang,Chao Wang
Phase transition will lead to abrupt change of thermoelectric material’s properties, which will have a negative influence on the application of thermoelectric device. Therefore, avoiding the phase transition of Ag 2 S is particularly important for its heat collection applications. In this work, we reported, for the first time, that Cu-Se co-alloying in Ag 2 S can suppress phase transition and improve thermoelectric properties. Specifically, different elements and compounds alloying in Ag 2 S samples were prepared, and their influences on the phase change behavior and thermoelectric performance stability of Ag 2 S are systematically studied. It is found that the free enthalpy decreases and the heat absorption peak disappears for the Cu-Se co-alloyed Ag 2 S sample. In addition, the average lattice thermal conductivity is greatly reduced, and the κ L of Ag 1.8 Cu 0.2 S 0.5 Se 0.5 is around 0.27 W m −1 K −1 from 330 K to 450 K. Therefore, a high ZT is obtained for Cu-Se co-alloyed Ag 2 S.
研究领域:
材料科学
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凝聚态物理
·
热电材料
·
无机非金属材料
·
功能材料
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高影响因子
International Journal of Minerals Metallurgy and Materials
·
2025
·Vol. 32
·期 12
·3072-3085
·
IF 7.2
Zhang Qian,Liu Bo,An Changcong,Li Qiong,Liu Jiling,Wei Siyu,Fan Jiaxing,Sun Zhe,Zhang Dichuan,Pulatov Bakhtiyor
The effect of heavy metals on the properties and hydration of blast furnace slag–cement composites (BFS-CC) remain unclear. In this study, two BFS-CC (denoted as DBFS-CC and WBFS-CC) were prepared by dry and wet grinding of BFS, respectively. The effect of Cu(II) on BFS-CC’s properties and hydration was investigated by adding representative copper contaminants (CuO, CuCl 2 , and CuS) to the composites. Adding 1.0wt% CuO and 0.5wt% CuS increased the 3-d compressive strength of DBFS-CC by 14.9% and 5.7%, respectively, but suppressed the 3-d strength of WBFS-CC. This trend reversed at 28-d curing, where adding 1.5wt% CuO, 2.0wt% CuCl 2 , and 1.5wt% CuS enhanced the compressive strength of WBFS-CC by 23.4%, 6.2%, and 13.6%, respectively, but adversely affected the strength of DBFS-CC. For 28-d hydration, adding CuCl 2 decreased the hydration degree of DBFS-CC but enhanced that of WBFS-CC. Adding CuO promoted the hydration degree of both composites, while adding CuS exhibited inhibitory effects. DBFS-CC immobilized CuCl 2 better due to a higher hydration degree, while WBFS-CC immobilized CuO and CuS better due to having finer unhydrated BFS particles and a denser matrix. This study not only focuses on the Cu(II) immobilization effect but also reveals the differential effects of Cu(II) species on the hydration process, providing novel insights into heavy metal interactions in BFS-CC systems and their safe disposal.
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ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.3
Tao Ding,Shunjie Shu,Yichen Gong,Zhensong Xu,Wen Xu,Jie Zhang,Lei Shi,Hui Sun,Yanhan Chen,Baitao Guo,Yujing Tan,Deliang Xu,Shu Zhang,Shaobin Wang,Hongqi Sun
Biomass waste utilization to produce desirable carbon-based catalysts opens new horizons for achieving carbon neutrality. Nevertheless, efficient manipulation of carbon support morphology and electronic structures of active sites remains a great challenge. By selecting adhesive-contained fiberboard waste as a C/N source and low-cost copper nitrate as a Cu donor, a well-designed carbon catalyst loaded with Cu atomic centers was constructed via a ZnCl2-assisted calcination strategy. Without adscititious N sources, the adhesive contributes to N doping into the carbon framework, further serving as Cu anchoring sites. Meanwhile, ZnCl2 adoption introduces abundant hierarchical pores, significantly improving the available surface area to enhance N doping and Cu dispersion. The as-synthesized catalyst (Cu ACs/aFC) exhibits impressive merits, such as a high specific surface area (∼1222 m2 g–1), homogeneously dispersed Cu sites with robust Cu–Nx configurations and tunable electronic structures, favorable surface hydrophilicity, and excellent electron migration, making it a promising candidate for catalytic reduction of nitroarenes and azo dyes. Taking 4-nitrophenol (4-NP) conversion into a high-value-added chemical (4-aminophenol) as an example, an impressive catalytic performance with a high TOF of 100.26 h–1 (∼2.1-fold that of its counterpart of Cu nanoparticle catalyst), as well as excellent reusability and long-term stability of up to 200 h, is achieved. Particularly, an efficient hydrogenation reduction toward a series of 4-NP analogues and azo dyes is demonstrated, displaying a huge application potential. Through selecting diverse metal precursors, the proposed strategy could be generalized to construct various biochar-based catalysts for advanced hydrogenation reactions.
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APPLIED SURFACE SCIENCE
·
2026
·
IF 6.9
Xiaofang Wen,Hongcan Lou,Zheng Li,Jiehao Xie,Zirui Qin,Xingkun Chen,Yuan Tan,Nian Lei,Wei Lu,Yunjie Ding
The development of efficient catalysts for the selective hydrogenation of dimethyl oxalate (DMO) to high-value oxygenates is of great industrial importance. This study presents a systematic investigation into the promotional effect of gallium (Ga) on Cu/SiO 2 catalysts for tailoring product selectivity in DMO hydrogenation. A series of Ga x Cu 30 /SiO 2 catalysts with varying Ga loadings (x = 0.5, 1, 3 wt%) were synthesized via the ammonia evaporation method. With a moderate Ga doping of 0.5 wt%, the Ga 0.5 Cu 30 /SiO 2 catalyst achieved an exceptional ethylene glycol (EG) yield of 74 %, which is three times higher than its Ga-free counterpart (23 %). Further increases in Ga loading to 1 and 3 wt% redirected the reaction pathway, steering the selectivity towards ethanol (ET, 81 %) and 2-methoxyethanol (MT, 54 %), respectively. Characterization by N 2 O titration, XRD, XPS, in situ FT-IR and H 2 -TPR revealed that Ga incorporation fine-tunes the synergy between metallic Cu 0 (for H 2 dissociation) and Cu + sites (for C=O bond polarization). Concurrently, the generated surface acid sites facilitate subsequent dehydration and hydrogenolysis steps. Consequently, the catalytic performance is directly correlated with the evolution of Cu valence states and surface acidity. This work provides a rational strategy for designing multifunctional catalysts for the selective synthesis of target chemicals from DMO.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 9.2
Zezhuang Wang,Yue Lyu,Baihe Guo,Yuchuan Feng,Haiyu Liu,Yan Jin,Juntian Niu
The efficient removal of ultra-low concentration methane from sources like coal mine ventilation air is crucial for mitigating greenhouse gas emissions. This study systematically investigates the effects of synthesis methods (impregnation, combustion, sol-gel, and co-precipitation) and Cu/Co ratios on the catalytic performance of Cu-Co/CeO 2 catalysts for ultra-low concentration methane combustion. Characterization results demonstrate the structural advantages of the optimal catalyst. XRD patterns confirm the successful formation of a CuCo 2 O 4 spinel phase. SEM images show a uniform morphology with minimal agglomeration. XPS analysis further reveals the coexistence of Cu 2+ /Cu + and Co 3+ /Co 2+ redox couples accompanied by abundant adsorbed oxygen species. Experiments demonstrate that the 1Cu-4Co/CeO 2 catalyst prepared by co-precipitation exhibits optimal low-temperature activity, with T 10 and T 90 values of 330 °C and 566 °C, respectively. Stability evaluations over 20 h at 500 °C show minimal activity decay, with the catalyst retaining 94.2% of its initial conversion. The superior performance is attributed to the synergistic redox interaction between Cu and Co, optimized surface oxygen mobility, and robust structural stability. This work provides an effective strategy for designing non-noble metal catalysts for ultra-low concentration methane purification.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Xiaosen Li,Chun Li,Yifan Fang,Xin Liang,Zhou Fang
Chemical agents present significant threat to international peace, security, and human health due to their potential toxicity. Therefore, developing a sensitive, rapid, and on-site detection method is of great importance. Herein, we developed a highly sensitive and selective glove-based electrochemical sensor based on a metal–organic-framework-modified screen printed electrode (SPE) for chemical agent marker detection. Layered copper benzene-1,3,5-tricarboxylate (Cu-BTC) was successfully constructed to modify screen-printed electrodes (SPE) for detecting electrically inactive ethyl methyl phosphonate (EMPA) and isopropyl methyl phosphonate (IMPA). Additionally, gold nanoparticles (AuNPs) reduced by plasma technology have been applied to create gold nanoparticle-encapsulated copper benzene-1,3,5-tricarboxylate-modified screen-printed electrode (Au@Cu-BTC/SPE) composites for detecting thiodiglycol (TDG). The large surface area and porous structure of Cu-BTC and Au@Cu-BTC enhance the target adsorption and ion diffusion and the efficient use of catalytic materials for rapid electron transfer and zero-distance catalysis. The limit of detection (LOD) was determined to be 4.13 × 10–16 M for EMPA, 7.46 × 10–12 M for IMPA, and 4.05 × 10–12 M for TDG. Following multiple cycles and extended exposure, the sensor demonstrated exceptional repeatability and stability. The response current of Cu-BTC to EMPA and IMPA decreased by 6.75% and 4.86%, and the peak value of Au@Cu-BTC to TDG decreased by 3.3% after 4 weeks, respectively. The peak current showed a good linear relationship with the concentrations of the three target substances, with R2 values all greater than 0.99. The interaction mechanism between the modified electrode and the targets was investigated by density functional theory (DFT) with the generalized gradient approximation of the PBE functional. The results showed that compared with other metal ions, Cu2+ could coordinate tighter with organophosphates. The established MOF-modified SPE integrated with a protective glove sensor was applied for the detection of real-world samples and demonstrated a broad spectrum of practical applications.
研究领域:
分析化学
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电化学
·
传感器与生物传感器
·
环境监测
·
安全与防御技术
·
纳米材料
·
金属有机框架（MOFs）
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PubMed
高影响因子
危险品化学品经营许可证（带存储）