Journal of Physical Chemistry C
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2021
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IF 4.126
Tianyou Chen,Wei Xiao,Zihao Wang,Pengfei Gan,Changfeng Yi,Zushun Xu
Noncovalent immobilization of discrete molecular species on polymer supports is a unique approach to engineer multifunctional cooperative catalysts. Here we devise a modular strategy for the construction of polymer-supported Cu/2,2,6,6-tetramethyl-1-piperidine-N-oxyl (TEMPO) catalytic systems by using hydrophobic interactions and aromatic stacking interactions. Polymer-supported Cu/TEMPO catalysts prepared by nanoprecipitation exhibit excellent catalytic activities for aerobic oxidation of benzyl alcohol, which can be tailored by the type of aromatic moieties, effective constituent ratios, and polymer compositions. We found that strong aromatic stacking interactions and the use of pyrene-containing polymers are crucial to enhance cooperativity. This modular strategy is promising for the immobilization of multifunctional cooperative catalysts with excellent catalytic activities and has potential for the engineering of other heterogeneous multifunctional catalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
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IF 19.503
Pengchao Ren,Weifeng Tu,Chanchan Wang,Sifan Cheng,Wenqi Liu,Zhenzhou Zhang,Yun Tian,Yi-Fan Han
This study investigated the Cu-CeO 2 interactions for CO hydrogenation to methanol by applying rate measurements, chemical titration/desorption, together with in-situ/operando spectroscopy techniques under realistic reaction conditions. Ce components were enriched in the surface region of Cu/CeO 2 catalysts while Ce 3+ and Ce 4+ atoms co-existed during CO hydrogenation. The ratio of Ce 3+ to Cu 0 in the surface region of catalysts increased linearly with the Ce content. The turnover rates of CH 3 OH formation increased as a single-valued function of the ratio, irrespective to the individual contact extent between Cu and CeO 2 clusters or Ce content in the Cu/CeO 2 catalysts, indicating that the Cu 0 -Ce 3+ sites pair acts as active sites for CO hydrogenation to methanol over Ce-CeO 2 samples. This study also unraveled that formyl and formate species, as reactive surface intermediates, were co-adsorbed on the Cu 0 -Ce 3+ sites, and their hydrogenation routes occurred concurrently for CH 3 OH formation during CO-H 2 reactions.
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SOLID STATE IONICS
·
2021
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IF 3.785
Yawen He,Zhongbin Ye,Mohamad Chamas,Moulay Tahar Sougrati,Pierre-Emmanuel Lippens
The silicon based composite Si/Cu-Zn(ox)/C was prepared by ball milling from Si microparticles , Cu-Zn nanopowder heated at air and carbon black. The composite is formed by Si submicrometer particles, Cu-rich Cu x Zn, CuO , ZnO and C nanoparticles . The two oxides are electrochemically active during the first discharge, improving the nanostructuration of the composite and providing Cu nanoparticles that enhance the electronic conductivity with Cu x Zn and C. The nanostructuration helps to buffer the volume variations due to Li-Si alloying reactions during cycling. The composite is further nanostructured during the first cycles as shown by XRD and electrochemical measurements. The material was tested as anode material for Li-ion batteries, providing a reversible capacity of 800 mAh.g −1 during 100 cycles at current of 300 mA.g −1 and a good rate capability. The reversible capacity is mainly due to Li-Si alloying reactions and is stable after few cycles while the solid electrolyte interphase is stabilized after about ten cycles as shown by electrochemical impedance spectroscopy .
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ENERGY & FUELS
·
2021
·
IF 3.605
Minghui Zhang,Yingying Liu,Yingming Zhu,Kejing Wu,Houfang Lu,Bin Liang
The complexation of metal ions and amines can mediate the chemical equilibrium and the thermal effect between amines and CO2, thus promoting the absorption and desorption of CO2 in amine absorbents. In this work, the effects of Cu(II) on the performances of CO2 absorption and desorption in the Cu(II)–MMEA (2-(methylamino)ethanol)–H2O system were studied. The thermal desorption results show that the temperature increase during CO2 absorption can be mitigated in the presence of Cu(II), and the desorption performance of CO2 can be obviously improved at 75–95 °C. Using the thermal desorption at 85 °C, the CO2 desorption efficiency of MMEA solution containing 0.1 M [Cu] is 16.4% higher than that without cupric ions, and the regeneration energy consumption is reduced by 25%. The electrochemical research results indicate that the electrode structure and temperature affect the electrolysis rate of anodic copper, and the temperature is the key factor to enhance the CO2 desorption rate. Only considering the decomposition voltage, the energy consumption of the absorbent regeneration is 0.5 GJ/t CO2 at 50 °C, which is much lower than that of the thermal desorption method. The anode current efficiency is always about 100%. Increasing the temperature can increase the cathode current efficiency. When nickel foam with a large specific surface area is used as the cathode, the current efficiency can be increased to 100% at 50 °C. The CO2 desorption is significantly improved in a Cu(II)-assisted MMEA–H2O system. The electrochemical method can achieve a desired desorption at a relatively low temperature and greatly reduce the energy consumption of amine absorbent regeneration.
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ACS Omega
·
2021
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IF 3.512
Ze Yuan,Lanlan Yang,Dongni Han,Guorong Sun,Chenyu Zhu,Yao Wang,Qiao Wang,Mikhail Artemyev,Jianguo Tang
High-efficiency photoluminescence quaternary hexagon Zn–Cu–In–S (ZCIS) nanoplatelets (NPls) have been synthesized by a two-step cation exchange method, which starts with the In2S3 NPls followed by the addition of Cu and Zn. It is the first time that In2S3 NPls are used as templates to synthesize ZCIS NPls. In this paper, the reaction temperature of In2S3 is essential for the formation of NPls. The photoluminescence wavelength of NPls can be tuned by adjusting the temperature of Cu addition. To enhance the stability of the resulting NPls and to improve their optical properties, we introduced Zn2+ and obtained ZCIS NPls by cation exchange on the surface. It is worth noting that the obtained ZCIS NPls show a shorter fluorescence lifetime than other ternary copper sulfide-based NPls. This work provides a new way to synthesize high-efficiency, nontoxic, and no byproduct ZCIS NPls.
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PubMed
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MINERALS ENGINEERING
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2021
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IF 4.765
Hai Yan,Bingqiao Yang,Huanyu Zhu,Pengliang Huang,Yangjia Hu
A small non-toxic compound dithiothreitol (DTT) was introduced as an environmental-friendly chalcopyrite depressant in Cu-Mo flotation separation. The separation performances were studied via flotation tests. The adsorption mechanism was explored by contact angle, Zeta potential and X-ray photoelectron spectroscopy (XPS) measurements. The flotation results manifested that DTT exhibited strong depression ability on chalcopyrite, but barely influenced the floatability of molybdenite. The contact angle and Zeta potential measurements indicated that DTT mainly adsorbed on chalcopyrite and rendered its surface hydrophilic, while it hardly adsorbed on molybdenite. XPS analysis confirmed that DTT might complex with Cu atoms on chalcopyrite surfaces via the thiol groups. This study demonstrated that DTT was a promising alternative for Na 2 S in Cu-Mo separation, which was more effective and environmentally compatible.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Ying Cai,Shihao Shen,Jinhong Fan
This study applied a mineral material of FeS to activate sulfite for efficient degradation of TTC in the presence of Cu(II) based on the identified complexation mechanism through UV–Vis spectra, FTIR spectroscopy and DFT calculation . pH plays an important role in TTC degradation and the initial pH of 6 and 7 were the divide in the contributions of FeS/sulfite oxidation and complex-precipitation. TTC-Cu(II) exhibits a superior promoting effect on the TTC degradation in FeS/sulfite system due to the improvement of TTC electron transfer reactivity and Fe(II) dissolution from FeS. Moreover, the formation of Cu(I) improved the recycling of Fe(II) from Fe(III). Dissolved oxygen-dependent free radicals’ generation was confirmed, and TTC degradation was mainly attributed to SO 4 ·− and ·OH. The characterization of FeS surface through XPS, XRD , SEM-EDS, Fe(II) deactivation tests, together with the comparison of pseudo-first-order rate constants for TTC degradation by FeS and ferrous ion supported the important role of surface and dissolved Fe(II) in sulfite activation . Furthermore, reasonable degradation pathways of TTC have been proposed according to the detected products by LC-MS. This work highlights the important role of pH, DO and Cu(II) complexation in sulfite activation and TTC degradation, furnishing theoretical support for further relevant studies.
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Molecular Catalysis
·
2021
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IF 5.062
Tianqinji Qi,Weizuo Li,Hong Li,Ke Ji,Shaoyun Chen,Yongchun Zhang
Revealing the origin of the enhanced performance on yttria (Y 2 O 3 ) promoted Cu/ZnO based catalyst for methanol synthesis via CO 2 hydrogenation is still challenging. To shed light upon the promotion effect of Y 2 O 3 modifier on binary Cu/ZnO catalyst for CO 2 hydrogenation reaction, a ternary Cu/ZnO/Y 2 O 3 catalyst was synthesized via a citric acid coordination-assisted strategy. The developed Cu/ZnO/Y 2 O 3 catalyst exhibited a remarkably higher Weight-time yeild of methanol (236.8 g MeOH g cat −1 ∙ h − 1 ) and methanol selectivity (81.1%) in comparison to Cu/ZnO catalyst (159.6 g MeOH g cat −1 ∙ h − 1 and 73.9%, respectively). Various characterizations results have uncovered the enhanced catalytic activity of Cu/ZnO/Y 2 O 3 catalyst for methanol synthesis was associated with small size and highly dispersed Cu species and abundant surface adsorption sites as well as more Cu-ZnO interfaces with strong interaction. Moreover, the Cu/ZnO/Y 2 O 3 catalyst displayed a superior weight-time yield of methanol with a time-on-stream of 100 h in comparison with classic Cu/ZnO catalyst. We anticipate that this basic design strategy will provide a novel alternative to expand opportunities to explore scalable, cost-effective catalysts for industrial methanol synthesis.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2021
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IF 4.098
Jun Wang,Jinjun He,Jinsheng Zhang,Zhiming Chen,Jinfu Liang,Lin Chen
In this work, a dual-functional Cu 2+ -based ensemble (2 S ·Cu 2+ ) was well designed and characterized. Then, the successional and discriminating sensing for CN − over other competitive species (H 2 PO 4 − and biothiols) was achieved based on the disaggregation of 2 S ·Cu 2+ ensemble and the deprotonation of imidazole NH of regenerated sensor S in aqueous solution, respectively. The visual sensing mechanism could be clearly demonstrated by 1 H NMR, HRMS and energy changes between the HOMO−LUMO band gaps. Furthermore, the reversibility and reusability of S and 2 S ·Cu 2+ upon alternating addition of CN − /H + and CN − /Cu 2+ were studied. Interestingly, the sequential sensing for biothiols (cysteine, glutathione and homocysteine) and CN − was also realized through spectroscopic methodology and test paper strips. This work may provide a feasible strategy to discriminate CN − over H 2 PO 4 − and biothiols with high selectivity and sensitivity through Cu 2+ -based ensembles.
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Journal of Physical Chemistry C
·
2020
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IF 4.189
Mengfan Liang,Ziyi Xiong,Yongmao Hu,Yingli Liu,Tao Shen,Shuhong Sun,Yan Zhu
In this article, we prepare corncob-like Cu–Ag and core–shell Cu@Ag bimetallic structures by controlling the concentration of Ag and Cu salts via a galvanic replacement reaction. Moreover, the structure evolution and electrical resistivity of the Cu–Ag corncob nanoparticle deposits were investigated upon heating up to 260 °C by experiments. Afterward, the effect of the distinctiveness and arrangement (such as core@shell, bifacial Janus, and nanowire structure) on the sintering behavior of Cu–Ag systems was investigated by molecular dynamics simulation. The results revealed that both the Ag–Cu ratio and the special structure in the initial stage as well as the sintering temperature play important roles in the morphological formation. Despite limited experimental observation of the structure evolution during sintering, the MD simulation provides a powerful tool to monitor the atom trajectory. The combined information from our experiment and molecular dynamics (MD) results will give guidelines for choosing the preferred structure of Cu–Ag systems when aiming at certain sintering properties.
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CARBOHYDRATE POLYMERS
·
2020
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IF 7.182
Fengxia Wang,Xu Ding,Xiaobo Niu,Xianyi Liu,Wei Wang,Ji Zhang
Although core-shell structure is favored by many applications, preparing it with green way is rarely been reported. Herein, a core-shell structured Cu@Pd-CS nanocomposite is greenly fabricated utilizing a natural chitosan and applied to glucose detection. As-obtained Cu@Pd-CS nanoparticles were characterized by transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and powder X-ray diffraction (XRD). When applied to glucose detection, the Cu@Pd-CS exhibits good stability, sensitivity and anti-interference. Moreover, it has a good linear relationship in glucose concentrations range of 0.1−1 mM with the sensitivity of 1.53 μA mM −1 cm −2 and 1−10 mM with the sensitivity of 23.00 μA mM −1 cm −2 . This work proves the practicability of building metal-based core-shell structure nanoparticles with green resources and glucose detection application.
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Journal of Materials Chemistry C
·
2020
·Vol. 8
·期 27
·9337-9344
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IF 7.059
Aili Wang,Lili Zhao,Hui Liu,Ziqian Zhou,Chengbo Li,Yong Xiang,Weijia Zhou,Feng Hao
The development of low-dimensional non-precious metal catalysts for the hydrogen evolution reaction (HER) is highly desired for clean energy utilization. Herein, we have reported a facile synthesis protocol of Cu–Mo–O (CMO) nanowires and nanosheets on Cu foam (CMOW/CF and CMOS/CF) through a one-step reaction of Cu nanowires with (NH4)6Mo7O24 solution directly under mild conditions. The final product morphology has been tuned by mechanical stirring. The as-synthesized CMOS/CF exhibits a low operating overpotential of 112 mV at a current density of 10 mA cm−2 with a high electrochemical active area of 25.1 mF cm−2 and excellent long-term stability in the 1 M KOH electrolyte. Moreover, by using the CMOS/CF as cathodic and anodic electocatalysts, a two-electrode electrolyzer capable of driving 10 mA cm−2 at a cell voltage of 1.69 V was achieved, along with promising stability. The high performance of the CMOS/CF can be attributed to higher electrochemical area and more Mo catalytic sites induced by mechanical stirring. This work provides a facile method for the synthesis and catalytic site regulation through a simple method of low-dimensional nanomaterials for the HER with relatively high electrochemical active area and catalytic activity.
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