Catalysis Science & Technology
·
2020
·Vol. 10
·期 15
·5149-5162
·
IF 5.721
Tongyang Song,Wei Chen,Yuanyuan Qi,Jiqing Lu,Peng Wu,Xiaohong Li
Achieving high catalytic performance with Cu-based catalysts is crucial for the hydrogenation of CO2-derived ethylene carbonate (EC) to simultaneously yield methanol (MeOH) and ethylene glycol (EG). Although Cu-based catalysts are widely studied for the target reaction, there are still some issues to be clarified. In this study, we prepared a 29.1 wt% Cu/SiO2-MHT catalyst by a modified hydrothermal method and successfully applied it to the hydrogenation of EC. In comparison with its three analogues having similar Cu loading and comparable Cu particle size but prepared by different methods, we found that the catalytic performance of the Cu/SiO2 catalysts, including the activity and the selectivity to MeOH, could be tuned by adjusting the Cu+/(Cu0 + Cu+) ratio via different preparation methods. As a result, the Cu/SiO2-MHT catalyst furnished 89% MeOH yield and 37.6 h−1 turnover frequency. To our best knowledge, these values are one of the highest among all heterogeneous Cu catalysts up to now. The results reveal that a cooperative effect exists between Cu0 and Cu+. When the Cu0 species are sufficient to activate H2, a more favorable formation of MeOH can be achieved with more Cu+ species and greater Cu+ surface areas. Furthermore, a greater amount of Lewis acid on the Cu/SiO2-MHT catalyst is also beneficial for MeOH formation.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Yanan Wang,Jiayu Ding,Qi Yin,Cheng Zhang,Yiqing Zeng,Song Xu,Qian Liang,Man Zhou,Zhongyu Li
This study developed a novel Cu@C/NCN-T composite for efficient photothermal catalytic CO 2 reduction. The composite, consisting of carbon-coated Cu (Cu@C) derived from Cu-BTC embedded in three-dimensional graphitic carbon nitride (NCN-T), was immobilized on the surface of carbonized wood (C-wood) floating on water, creating a triphase system (CO 2 , H 2 O, and catalyst). The optimized composite demonstrated remarkable CO 2 photothermal reduction performance, achieving a rate of 31.3 μmol·g −1 ·h −1 . This performance surpassed that of pure NCN-T and Cu@C by 1.6 and 3.8 times, respectively. The combination of Cu and carbon materials endowed Cu@C/NCN-T with excellent light-absorption properties, resulting in a photothermal effect that elevated the surface temperature and facilitated the catalytic reaction . Furthermore, the Schottky junction formed between Cu@C and NCN-T promoted the separation of electron-hole pairs, with Cu@C acting as charge channels. A charge transfer mechanism was proposed to explain these findings. This catalyst engineering approach holds promise for the development of efficient non-noble metal catalysts for rapid CO 2 photothermal reduction.
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Energy Storage Materials
·
2024
·
IF 18.9
Jing Peng,Bihua Hu,Zhitong Li,Xiongwei Zhong,Junwei Shi,Shuyu Cui,Xingzhu Wang,Baomin Xu
Dual-metal single-atom catalysts with heteronuclear active sites exhibit superior oxygen catalysis performance than their single-atom counterparts, facilitating the practical applications in advanced electrochemical energy devices. Herein, a Fe-Cu dual-metal single-atom catalyst with Fe-N 6 and Cu-N 1 S 2 coordination environment (FeCu-DSAs/NSC) is reported. Due to the synergism of bimetallic active sites and asymmetric heteroatom coordination, the resultant FeCu-DSAs/NSC displays better bifunctional catalytic performance (a small potential gap between the E η10 and E 1/2 , ΔE=0.647 V) when compared with the counterparts (Pt/C+IrO 2 and Cu-ISAs/NSC), as well as surpassing most of bifunctional metal atom-based catalysts reported to date. As expected, FeCu-DSAs/NSC based rechargeable zinc-air battery shows remarkable superiority than commercial Pt/C+IrO 2 benchmark, resulting in a high peak power density (230.66 mW cm −2 ), open-circuit voltage (1.464 V) and long-term cycling stability (up to 350 h at 10 mA cm −2 ).
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Peng Wang,Wei Nong,Yan Li,Hao Cui,Chengxin Wang
Although the electrochemical nitrogen reduction reaction (NRR) is regarded as a promising alternative to the Haber–Bosch process, it still suffers from the poor activity and low selectivity. Herein, we propose a powerful strategy to simultaneously boost the activity and selectivity by introducing strain engineering into the design of NRR electrocatalysts. The strain-engineered electrocatalysts consisted of monodisperse CuAu@Cu core-shell nanoparticles with controllable Cu skin via one-pot solvothermal process. Among them, electrocatalysts with about 2 layers of atomic Cu skin (CuAu@2LCS) achieve the highest NH 3 yield rate (33.9 μg NH3 h −1 mg cat. −1 ) and Faradic efficiency (24.1 %) at –0.2 V vs. RHE in 0.1 M HCl. Density functional theory (DFT) calculations reveal that owing to the unique structure of bimetallic alloys with the ultra-thin Cu skins, tensile strain and favorable ligand effect work together and tune the surface electronic structure of electrocatalysts, which not only strengthen N 2 affinity but also suppress the competitive HER process.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Yonglong Huang,Zhengkang Duan,Chuan Li,Tian Qiu
The catalytic dehydrogenation of diethanolamine to prepare iminodiacetic acid has attracted considerable research interest. However, the lack of understanding of the structure-activity relationship of the reaction can present a challenge to the control of the catalytic behavior. Concurrently, improving the catalytic performance and reducing the cost have also become urgent issues that require resolution. This work examined the catalytic mechanism of several Cu-Ni X /ZrO 2 catalysts, differing in Cu/Ni ratios, prepared by H 2 reduction, in the context of DEA dehydrogenation to elucidate the structure-activity connection and probable reaction mechanism. Subsequently, a strategy has been put out to generate metal (Ni and Co)-doped copper-zirconium catalysts using the co-precipitation-hydrazine hydrate reduction process. The synergistic effect between metals was combined with the improvement of the surface reaction of the catalyst by hydrazine hydrate through a more efficient preparation method, thereby enhancing the catalyst's overall performance. The representative catalyst Cu-Ni/ZrO 2 required a hydrazine hydrate reduction temperature and time of 40 °C and 30 min, and after 65 min of reaction, it exhibited a high conversion rate (96.3 %) and yield (93.7 %), and after five cycles, both the conversion rate and yield exceeded 85 %. Various characterization techniques have confirmed that Ni doping induced an alloying effect and a size effect. Additionally, the hydrazine hydrate reduction method was discovered to augment the specific surface area, surface hydroxyl groups, hydrophilicity, and optimize the pore size distribution of the catalyst while also regularizing its morphology, thereby significantly enhancing the activity and stability of the metal-doped copper-zirconium catalyst. This paper discussed the correlation between catalyst structure and reaction performance, as well as the catalytic conversion mechanism, which is anticipated to provide a novel reference for the preparation, performance control, and potential applications of dehydrogenation catalysts.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Li-Na Song,Li-Jun Zheng,Xiao-Xue Wang,Yi-Feng Wang,Yue Wang,Shuang Liang,Ji-Jing Xu
The design of highly efficient electrocatalysts is a promising strategy to improve the electrochemical kinetics of Li–CO2 batteries. However, electrocatalysts usually aim to reduce the energetic barrier for the corresponding electrochemical reactions; little attention has been given to modulating the kinetics that directly determine the local concentration of reaction molecules surrounding catalysts. Herein, we present a systematic study on the role of Li+ reunion on the improvement of reaction kinetics in Li–CO2 batteries with a Cu cone cathode. Specifically, this local, geometry-driven tip effect can enrich the local electron concentration to facilitate Li+ ions diffusion from the bulk electrolyte to the surface of catalyst, leading to boosted catalytic performance. Further studies demonstrate that Cu(II/I) as a solid redox mediator dominates the reversible bulk redox reactions in a Cu cone cathode, which acts as an electron–hole transfer agent and permits the efficient reduction and oxidation of solid Li2CO3, contributing to an accessible theoretical discharge voltage, low charge potential below 3.2 V, impressive rate capability, and a long cycling stability (333 days) for Li–CO2 batteries. The exploitation of the sharp-tip enhancement effect and dynamic creation of catalytic active sites is expected to become routine practice in future mechanistic studies for metal-air batteries.
研究领域:
电化学
·
材料科学
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Journal of Environmental Sciences
·
2020
·
IF 4.302
Sijia Qian,Shengyan Pu,Ying Zhang,Peng Wang,Yingchen Bai,Bo Lai
TiO 2 /graphene oxide (GO) as photocatalyst in the photo-degradation of multitudinous pollutants has been extensively studied. But its low photocatalytic efficiency is attributed to the high band gap energy which lead to low light utilization. Cu-TiO 2 /GO was synthesized via the impregnation methods to enhance the catalytic performance. The Cu-TiO 2 /GO reaction rate constant for photo-degradation of pollutants (tetracycline hydrochloride, TC) was about 1.4 times that of TiO 2 /GO. In 90 min, the removal ratio of Cu-TiO 2 /GO for TC was 98%, and the maximum degradation ratio occurred at pH 5. After five cycles, the removal ratio of Cu-TiO 2 /GO still exceeded 98%. UV–visible adsorption spectra of Cu-TiO 2 /GO showed that its band gap was narrower than TiO 2 /GO. Electron paramagnetic resonance (EPR) spectra test illustrated the generation rate of •O 2 − and •OH was higher in Cu-TiO 2 /GO system than TiO 2 /GO and TiO 2 system. The contribution sequence of oxidative species was •O 2 − > holes (h + ) > •OH in both TiO 2 /GO and Cu-TiO 2 /GO system. Interestingly, the contribution of •OH in Cu-TiO 2 /GO was less than that in TiO 2 /GO during the photo-degradation process. This phenomenon was attributed to the better adsorption performance of Cu-TiO 2 /GO which could reduce the accessibility of TC to •OH in liquid. The enhanced non‑hydroxyl radical contribution could be attributed to that the more other active species or sites on (nearby) the surface of Cu-TiO 2 /GO generated after doping Cu. These results provide a new perspective for the tradition metal-doped conventional catalysts to enhance the removal of organic pollutants in the environment.
研究领域:
环境科学
·
材料科学
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PubMed
高影响因子
TALANTA
·
2020
·
IF 5.339
Zhentao Li,Zhenkun Mao,Wei Zhou,Zilin Chen
Metal-organic frameworks (MOFs) are a novel class of porous nanomaterials composed of metals and organic linkers that have been used in many fields. A novel stereoselective stationary phase for capillary electrochromatography (CEC) has been developed in this work by employing a biodegradable, easier-to-prepare and green homochiral MOFs (Cu-SD), which composed of octakis-[6-deoxy-6-(3-mercaptopropanoic sodium)]-γ-cyclodextrin (SD, sugammadex) and transition metal ion (Cu 2+ ) supported by polydopamine as linker. The modified capillary was characterized by scanning electron microscopy (SEM), X-ray spectrometry (XRD), energy dispersive (EDS) and Fourier transform infrared spectroscopy (FT-IR). The Cu-SD modified capillary column exhibited outstanding chiral recognition separation for five Dns-DL-amino acids (the DL-forms of phenylalanine , leucine , valine , threonine , serine). In addition, the modified column showed excellent stability and reproducibility. The relative standard deviations (RSDs) of the retention time for intra-day (n = 5) and inter-day (n = 3) and between columns (n = 3) enantioseparations were less than 0.27, 1.45 and 4.88%, respectively. Conceivably, this new-type of γ-CD-MOF represents a useful chiral stationary phase in electrochromatographic separations, and it has great potential in chiral separation field.
研究领域:
分析化学
·
材料科学
·
药物化学
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CERAMICS INTERNATIONAL
·
2022
·
IF 5.532
Xinyuan Lyu,Zhengxin Li,Jingjing Jin,Yuze Xue,Chaogang Yu,Luchao Ren,Mingwei Zhang,Hongqing Zhou
In this study, we prepared a novel series of Li 2 x Cu 1- x MoO 4 ( x = 0.02, 0.04, 0.06, 0.08, and 0.10) microwave ceramics. The dynamic sintering behavior, crystal phases, micro-morphologies, and dielectric properties of the samples were studied. The substitution of Li + contributed to refining the crystal grain size, promoting the densification of microstructure, and enhancing the quality factor. Due to different valence substitutions, Cu + ions were created, which were verified by X-ray photoelectron spectroscopy (XPS) and Raman experiments. In addition, the Raman shift, full width at half maximum (FWHM) value of the A 1g peak, and crystal microstrains were analyzed to gain a mechanistic understanding of the influence of structure on the dielectric properties . When x = 0.08, the Li 2 x Cu 1- x MoO 4 ceramic sintered at 675 °C exhibited optimal comprehensive properties with ε r = 8.17, Qf = 68 476 GHz, and τ f = −25 ppm/°C, and good chemical stability between the ceramic and Al electrode was also achieved. These promising properties make Li 2 x Cu 1- x MoO 4 ( x = 0.08) more suitable for ultra-low temperature co-fired ceramic (ULTCC) applications.
研究领域:
材料科学
·
电子工程
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Zhiqun Xie,Jiali Zhou,Jinnan Wang,Corvini Philippe François-Xavier,Thomas Wintgens
Novel Fenton-like catalyst γ-Cu-Al 2 O 3 -Bi 12 O 15 Cl 6 with electron-poor Cu centre and electron-rich Bi centre was synthesized for selective degradation of phenolic compounds. Different from electron-rich Cu centre catalysts, the electron-poor Cu centre, which was induced by high electronegativity of Bi, could facilitate the formation of σ-Cu-ligand with phenolic compounds. On one hand, H 2 O 2 could directly oxidize σ-Cu-ligand to HO-adduct radicals with the generation of OH. Meanwhile, Cu(II) in the σ-Cu(II) complexes could be reduced to Cu(I) by oxidization of the HO-adduct radicals to hydroxylation products. Such reaction not only prevented Cu(II) from oxidizing H 2 O 2 to HO 2 /O 2 − but also enhanced the redox cycle of Cu(II)/Cu(I), which improved the catalytic activity and H 2 O 2 utilization. On the other hand, although the σ-Cu-ligand was gradually decreased with the decrease of phenolic compounds, dual-reaction centre played the dominant role in catalytic reaction . In addition, large amounts of oxygen vacancies (OVs) are formed in Bi 12 O 15 Cl 6 during the calcining process (BiOCl→Bi 12 O 15 Cl 6 ) , which can also increase the generation of OH. Thus, both electron-rich Bi center and OVs could still reduce H 2 O 2 to · OH for organics degradation even without the formation of σ-Cu-ligand. Being attributed to the synergistic effect of σ-Cu-ligand, dual-reaction centre and OVs mentioned above, γ-Cu-Al 2 O 3 -Bi 12 O 15 Cl 6 achieved high catalytic activity for phenolic compounds degradation and utilization efficiency of H 2 O 2 (η). In addition, various analytic methods (XPS, TPR, FT-IR, Raman, EPR and solid-state EPR) were used to prove the synergistic effect of the electron-poor/rich centre, σ-Cu-ligand and OVs of catalyst.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Zhenjiang Li,Chenghai Gao,Huimin Zhao,Alan Meng,Shiqi Ding,Xuehua Wang,Shaoxiang Li
Exploration of new non-precious metal catalysts for highly efficient oxygen reduction reaction (ORR) is essential for sustainable energy utilization technologies. Herein, porous biomass-derived carbon modified by Cu, N co-doping and Cu nanoparticles was synthesized by hydrothermal followed pyrolysis strategy, and used for electrocatalytic ORR. The optimized Cu/Cu-N-C catalyst exhibits large surface area (235.91 cm 3 g −1 ) and hierarchical pore structure . Benefiting from the above factors, the Cu/Cu-N-C catalyst performs a high onset potential (E onset , 0.947 V vs. reversible hydrogen potential (RHE)) and a half-wave potential (E 1/2 , 0.875 V vs. RHE) in 0.1 M KOH solution. The calculated electron transfer number of 3.92 suggests the near-four-electron ORR process. Besides, the Cu/Cu-N-C catalyst also performs extraordinary stability and higher methanol tolerance than Pt/C. In addition, the assembled Zn-air battery based on the optimized Cu/Cu-N-C catalyst exhibits a higher power density of 150.7 mW cm −2 than the that of Pt/C-based battery. This work put forward a newfangled method to fabricate efficient ORR catalyst by loading active component on biomass-derived carbon, which follows the sustainable development concept, and provides a profitable reference for designing nonprecious metal carbon-based ORR electrocatalyst .
研究领域:
能源材料科学
·
电催化
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ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Ze Chai,Chuanhai Jiang
The electrochemical/chemical growth of porous (Ni,Co,Cu)(OH) 2 was reported based on the corrosion behaviors of Ni-Co-Cu films in neutral salt spray . The films prepared by using electrodeposition were ternary solid solution alloys with a simple phase structure, strong texture, nanoscale grains, large microstrain and a large number of crystal defects . The unique microstructures coupled with extensive ion diffusion during the subsequent corrosion process facilitated the formation of ternary hydroxides with uniform and porous nanostructures . The ternary hydroxides composed of Ni-/Co-dominant hydrotalcite-like and Cu-dominant orthorhombic (Ni,Co,Cu)(OH) 2 could be efficiently prepared by motivating the transformation from oxide to hydroxide. The binder-free (Ni,Co,Cu)(OH) 2 electrode exhibited a high specific capacitance of 1738 F g −1 at a current density of 20 A g −1 and decent cycling stability. The electrochemical/chemical growth mode, uniform porous nanostructures and nature of the ternary hydroxides could account for the superior electrochemical performances. This work proposed a simple and green approach to prepare multicomponent hydroxides as novel electrode materials for rechargeable batteries and hybrid supercapacitors .
研究领域:
材料科学
·
电化学
·
储能技术
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纳米材料
·
腐蚀科学
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高影响因子
危险品化学品经营许可证（带存储）