ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Lei Xiao,Chaowei Yuan,Peng Chen,Yongyi Liu,Jianping Sheng,Shihan Zhang,Fan Dong,Yanjuan Sun
Due to the intrinsic chemically inert CO2 with the dissociation energy of C═O bond as high as 750 kJ mol–1, low efficiency and selectivity have become the most significant restraints for the practical application of photocatalytic CO2 reduction. Renewing the electronic structure of adsorbed CO2 on the catalyst surface through a rational catalyst design is crucial to achieving performance improvement. Herein, we prepared ZnIn2S4 and Cu-substituted ZnIn2S4 containing both Lewis acid and Lewis base sites as a model system for investigating the activation of CO2 by M–S chemical bonds (M represents a metal site). The Cu–S chemical bond can effectively activate CO2 as a vital electron channel and lower the Gibbs free energy for generating the essential intermediate *COOH. Besides, the Cu0.7-ZnIn2S4 sample displays 74.8% selectivity for reducing CO2 to CO with a rate of 47.2 μmol g–1 h–1, roughly 7.14 times that of ZnIn2S4.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
PLASMA CHEMISTRY AND PLASMA PROCESSING
·
2023
·Vol. 43
·期 6
·1963-1978
·
IF 3.6
Lv Huan,Liu Xinyuan,Hao Yingzi,Yi Yanhui
The industrial utilization of methane to methanol is based on the indirect pathway with syngas as an intermediate product, but the reaction conditions are very harsh and the costs in equipment and operations are extremely high. Therefore, the direct oxidation of methane to methanol (DOMTM) under mild conditions is more desirable. In this paper, coupling of non-thermal plasma and Cu–zeolite (Cu–ZSM-5 and Cu–S-1) catalysts have been studied for DOMTM. The effect of Si/Al ratios (Cu–ZSM-5 and Cu–S-1 catalysts) on the reaction performance has been investigated. Cu–S-1 catalyst exhibited the best catalytic performance, i.e., 5.8% methane conversion and 50.6% methanol selectivity. The employed catalysts have been characterized by XRD, UV–Vis, XPS and FT-IR. The results show that Cu–ZSM-5 catalysts with high Si/Al ratio are conducive to the formation of isolated Cu 2+ species, and Cu–S-1 catalyst exhibits the most abundant isolated Cu 2+ species. Furthermore, Cu–S-1 catalyst shows the most abundant O ads species. The plentiful surface silicon defects on S-1 is the reason why Cu–S-1 catalyst shows the most abundant isolated Cu 2+ and O ads species, and these two species are interdependent to form a Si–O–Cu species, which may be the active site for DOMTM. Based on these findings, the possible catalytic mechanism was proposed.
研究领域:
化学工程
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催化化学
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DOI
高影响因子
Energies
·
2024
·Vol. 17
·期 6
·1449
·
IF 3
Qiong Li,Yu Wang,Ganghui Wei,Xiaorong Fang,Ni Lan,Yonggang Zhao,Qiming Liu,Shumei Lin,Deyan He
The preparation of composite carbon nanomaterials is one of the methods for improving the electrochemical performance of carbon-based electrode materials for supercapacitors. However, traditional preparation methods are complicated and time-consuming, and the binder also leads to an increase in impedance and a decrease in specific capacitance. Therefore, in this work, we reduced Ni-Cu nanoparticles on the surface of nitrogen-doped carbon nanofibers (CNFs) by employing an electrostatic spinning method combined with pre-oxidation and annealing treatments. At the same time, Ni-Cu nanoparticles were vulcanized to Ni–Cu–S nanoparticles without destroying the structure of the CNFs. The area-specific capacitance of the CNFs/Ni–Cu–S–300 electrode reaches 1208 mF cm−2at a current density of 1 mA cm−2, and the electrode has a good cycling stability with a capacitance retention rate of 76.5% after 5000 cycles. As a self-supporting electrode, this electrode can avoid the problem of the poor adhesion of electrode materials and the low utilization of active materials due to the inactivity of the binder and conductive agent in conventional collector electrodes, so it has excellent potential for application.
研究领域:
材料科学
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能源存储
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Ruihong Guo,Yujuan Zhang,Xiutang Zhang,Hong Yang,Tuoping Hu
The development of efficient bifunctional catalysts is the key technology to replace oxygen evolution reaction (OER) with hydrazine oxidation reaction (HzOR) with lower theoretical potential to achieve high efficiency and energy-saving hydrogen production . In this work, the Co 0·52 Cu 0·48 /Cu@S–C (−1.3 V) composite with flower-like array was prepared by two-step electrodeposition coupled pyrolysis method. The electrochemical measurements showed that the driving voltages of the optimal composite for HzOR and hydrogen evolution reaction (HER) are respectively −118 mV and 47 mV at a current density (j) of 10 mA cm −2 . The excellent performance of Co 0·52 Cu 0·48 /Cu@S–C (−1.3 V) composite is attributed to the fact that the flower-like structure exposes more active areas and facilitates the diffusion of electrolyte, the strong electron interaction between Co 0·52 Cu 0·48 /Cu and S –C substrate, which can be verified by X-ray photoelectron spectroscopy (XPS), enhances the electrical conductivity , the Co 0·52 Cu 0·48 /Cu heterogeneous interface reduces the water dissociation barrier and facilitates the dehydrogenation kinetics of N 2 H 4 determined by density functional theory (DFT) calculations. Due to the excellent performance of Co 0·52 Cu 0·48 /Cu@S–C (−1.3 V), the overall hydrazine splitting (OHzS) electrolytic cell was constructed with Co 0·52 Cu 0·48 /Cu@S–C (−1.3 V) as electrodes. The results showed the voltages required by the cell are 36, 210 and 282 mV at the current density values of 10, 100 and 200 mA cm −2 respectively, showing that Co 0·52 Cu 0·48 /Cu@S–C (−1.3 V) can be used for energy-saving hydrogen production by hydrazine assisted water electrolysis.
研究领域:
材料科学
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电化学
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催化科学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Xuli Hu,Zhen Zhang,Zhenyao Li,Yushan Wu,Wei Wei,Yao Wang,Junchen Xu,Mingyue Ding
Regulating oxidation state of Cu-based chalcogenides catalysts during electrolysis is of great significance for efficient CO 2 electrochemical reduction reaction (CO 2 RR) to methanol, which still remains a dramatic challenge. Herein, we construct a heterogeneous Cu 3 VS 4 /CuS electrocatalyst (denoted as CuV x S), in which the in-situ growing Cu-S-V bonds avoid the accumulated electrons on oxidized Cu sites and inhibit the deep reduction of CuS to metallic Cu during electrolysis, maintaining stable and abundant reactive Cu + /Cu 2+ species to promote CO 2 RR performance to methanol. By this design, the CuV 0.1 S catalyst achieves an ultrahigh methanol selectivity of 79.8 %. In-situ FTIR measurement reveals that the synergistic effect of Cu + /Cu 2+ species and Cu-S-V bonding facilitates the *CO adsorption and the subsequent *CO hydrogenation process, which improve the generation of *CHO and *OCH 3 intermediates for enhanced methanol selectivity. This work provides a new insight into stabilizing high oxidation state of Cu-based electrocatalyst to maintain sufficient active sites for CO 2 RR.
研究领域:
电化学
·
催化材料科学
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DOI
高影响因子
Matter
·
2023
·
IF 18.9
Shilin Zhu,Wei Wu,Zheng Li,Jianlin Luo
Lee et al. report that the compound LK-99, with a chemical formula of Pb 10-x Cu x (PO 4 ) 6 O (0.9 < x < 1.1), exhibits room temperature superconductivity under ambient pressure. In this study, we investigated the transport and magnetic properties of pure Cu 2 S and LK-99 containing Cu 2 S. We observed a sharp superconducting-like transition and a thermal hysteresis behavior in the resistivity and magnetic susceptibility. However, we did not observe zero resistivity below the transition temperature. We argue that the so-called superconducting behavior in LK-99 is most likely due to a reduction in resistivity caused by the first-order structural phase transition of Cu 2 S at around 385 K, from the hexagonal structure phase at high temperature to the monoclinic structure phase at low temperature.
研究领域:
凝聚态物理
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材料科学
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超导电性
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相变物理
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电子输运性质
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DOI
高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2023
·Vol. 120
·期 42
·e2312091120
·
IF 11.1
Xia Lin,Junwei Zhang,Huihui Yan,Jiaxi Xu,Zhonghao Miao,Guangchang Shu,Shuyuan Zhao,Tianyuan Zhang,Haoxiang Yu,Lei Yan,Liyuan Zhang,Jie Shu
Metal-sulfur batteries have received great attention for electrochemical energy storage due to high theoretical capacity and low cost, but their further development is impeded by low sulfur utilization, poor electrochemical kinetics, and serious shuttle effect of the sulfur cathode. To avoid these problems, herein, a triple-synergistic small-molecule sulfur cathode is designed by employing N, S co-doped hierarchical porous bamboo charcoal as a sulfur host in an aqueous Cu-S battery. Expect the enhanced conductivity and chemisorption induced by N, S synergistic co-doping, the intrinsic synergy of macro-/meso-/microporous triple structure also ensures space-confined small-molecule sulfur as high utilization reactant and effectively alleviates the volume expansion during conversion reaction. Under a further joint synergy between hierarchical structure and heteroatom doping, the resulting sulfur cathode endows the Cu-S battery with outstanding electrochemical performance. Cycled at 5 A g−1, it can deliver a high reversible capacity of 2,509.8 mAh g−1 with a good capacity retention of 97.9% after 800 cycles. In addition, a flexible hybrid pouch cell built by a small-molecule sulfur cathode, Zn anode, and gel electrolytes can firmly deliver high average operating voltage of about 1.3 V with a reversible capacity of over 2,500 mAh g−1 under various destructive conditions, suggesting that the triple-synergistic small-molecule sulfur cathode promises energetic metal-sulfur batteries.
研究领域:
材料科学
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电化学
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能源存储
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产品关联
DOI
PubMed
高影响因子
FUEL
·
2025
·
IF 7.5
Honglin Li,Xin Zhang,Yuanyuan Wen,Jingyuan Li,Yu Liu,Hongjun Mao,Hongman Sun,Jingbin Zeng,Zifeng Yan
Sulfur-doped copper (S-doped Cu) was regarded as an efficient catalyst for formate in CO 2 electrochemical reduction reaction (CO 2 RR), but the selectivity and current density are still unsatisfied due to the hydrogen evolution reaction (HER) and CO generation pathway. Herein, S-doped Cu nanoparticles were synthesized by in-situ reduction of the constructed Cu-thioamide coordination polymers, exhibiting impressive performance for formate production in the CO 2 RR process. Particularly, the CuBr-thiobenzamide (TBA) coordination polymers derived S-doped Cu nanoparticles (CuBr-TBA-R) achieve a formate Faradaic efficiency of 84.4 % with current density of formate to 6.7 mA cm −2 . The characterization results indicate these generated S-doped Cu nanoparticles are uniform with the particle size of 20–30 nm exposed a large amount of Cu (100) facets due to the coordination of thioamide molecules and presence of Br - and I - in electrolyte. The morphological characteristics and strong affinity for oxygen is the reason of higher formate selectivity and current density. This finding reveals the characterizations of efficient S-doped Cu catalysts for formate and provide a controllable approach to prepare these catalysts.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
SOLID STATE SCIENCES
·
2023
·
IF 3.5
Huadong Liu,Hao Sun,Du Ke Zhen,Cheng Jing liang,Sun XiaoYu
Monoclinic bismuth vanadate (m-BiVO 4 ) is a well-known photocatalytic material. However, its poor charge transport and photogenerated electron hole rapid recombination limit the application of m-BiVO 4 . In this paper, we successfully constructed a novel copper-sulfur co-doped carbon quantum dots (Cu, S-CQDs)/BiVO 4 nanocomposite through a facile and efficient route, which significantly improved the photocatalytic performance of BiVO 4 . The physicochemical properties of Cu, S-CQDs and Cu, S-CQDs/BiVO 4 samples were studied by various characterization. It was concluded from the degradation experiments that the photocatalytic degradation rate of rhodamine B reaches 99% in 60 min under natural light. The degradation curve compounds the quasi-primary kinetic model, and the kinetic coefficient of degradation is 0.07831 min −1 , which is 5.37 times than that of pure BiVO 4 . Moreover, the free radical scavenging experiments reveal that the hole and superoxide radicals play a major role in the photocatalysis process. After four cycles, the activity of photocatalyst exhibits high stability, which is extremely important for the photocatalytic process. In the summery, the prepared Cu, S-CQDs/BiVO 4 has many advantages, such as environmental-friendly, low cost and a wide range of applications.
研究领域:
材料科学
·
环境科学
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产品关联
DOI
高影响因子
TALANTA
·
2021
·
IF 6.057
Hui Huang,Meini Li,Mingwei Hao,Liangli (Lucy) Yu,Yongxin Li
A selective and sensitive colorimetric strategy for sulfide analysis was developed using GMP-Cu nanozymes with a laccase-like activity. This research discovered for the first time that sulfide could significantly enhance the catalytic activity of the GMP-Cu nanozymes by about 3.5 folds. The enhanced laccase activities duo to two reasons. First, Cu 2+ in GMP-Cu nanozymes was reduced to Cu + . The other reason was the formation of Cu–S bond which was beneficial to accelerate the electron transfer rate to improve catalytic activity. Therefore, this method showed an excellent selectivity for sulfide. And it had a linear relationship in the sulfide concentration range of 0–220 μmol/L with a detection limit of 0.67 μmol/L. Furthermore, the proposed method was successfully applied to examine sulfide in the food systems. This new method may be used in sulfide detection to improve food quality and safety.
研究领域:
分析化学
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食品科学
·
纳米技术
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产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2024
·
IF 4.4
Huadong Liu,Hao Sun,XiaoYu Sun,Jing liang Cheng
This paper presents a novel tubular microreactor immobilized a photocatalyst to overcome the limitations of low light utilization and the challenges associated with catalyst recovery in traditional photocatalysis reactors. The copper-sulfur co-doped carbon quantum dots (Cu, S-CQDs)/bismuth vanadate (BiVO 4 ) composites were successfully immobilized on the inner surface of the microreactor channel through the sol–gel process. The catalytic layer in the microreactor enlarged the specific surface area and facilitated the mass transfer. Meanwhile, it also greatly reduced the consumption of chemical supplies and eliminated the need for recycling the photocatalyst. The morphology and structural features of the catalytic layer were studied by characterization. Then the photocatalytic performance of the microreactor was evaluated by photocatalytic degradation of Rhodamine B. The photocatalytic kinetics of the photocatalytic reaction in the microreactor was 0.60925, which was 10.49 times greater than that in the macroscopic system. The results showed that the microreactor led to a significant improvement in degradation efficiency. The reproducibility experiments conducted on the microreactor system further demonstrate its excellent stability. In short, integrating the beneficial properties of microreactors with Cu, S-CQDs/BiVO 4 exhibits highly promising prospects of photocatalytic applications.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
高影响因子
Small
·
2023
·Vol. 19
·期 52
·2304718
·
IF 13.3
Zhi Li,Zhengyang Zhou,Jiawei Zhang,Chenxi Zhu,Pengfei Qiu,Tingting Deng,Fangfang Xu,Lidong Chen,Xun Shi
Materials with low thermal conductivity have received significant attention across various research fields, including thermal insulation materials, thermal barrier coatings, and thermoelectric materials. Exploring novel materials with intrinsically low thermal conductivity and investigating their phonon transport properties, chemical bonding, and atomic coordination are crucial. In this study, a novel ternary sulfide is successfully discovered, Cu 2 ZrS 3 , which is achieved by introducing copper ions into both the interlayer and intralayer of ZrS 2 . The resulting structure encompasses various coordination forms within each layer, such as [CuS 4 ], [ZrS 6 ], and [CuS 3 ], leading to pronounced phonon anharmonicity induced by the asymmetric bonding of tri-coordinated Cu atoms within the [ZrS 6 ] layer. As a result, Cu 2 ZrS 3 exhibits intrinsically low lattice thermal conductivity ( κ L ) of about 0.83 W m −1 K −1 at 300 K and 0.35 W m −1 K −1 at 683 K, which are in the exceptionally low level among sulfides. In comparison to the conventional approach of inserting guests between layers, the substitution of atoms within layers provides a novel and effective strategy for designing low κ L materials in transition metal dichalcogenides (TMDCs).
研究领域:
材料科学
·
热电学
·
固态化学
·
声子物理
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DOI
高影响因子
危险品化学品经营许可证（带存储）