JOURNAL OF CATALYSIS
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2021
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IF 7.92
Yue Ma,Songqi Cheng,Xiaodong Wu,Tongxi Ma,Liping Liu,Baofang Jin,Minghan Liu,Jianbo Liu,Rui Ran,Zhichun Si,Duan Weng
To improve the hydrothermal durability of Cu-SSZ-13 selective catalytic reduction (SCR) catalyst, a thin Al 2 O 3 modification layer was coated on the external surface of Cu-SSZ-13 by a chemical liquid deposition (CLD) method. The high-temperature SCR activity of the Al-modified Cu-SSZ-13 can be maintained upon 750–800 °C hydrothermal aging, and over-oxidation of NH 3 is largely inhibited. Based on H 2 -TPR and EPR results, it is revealed that CuAl 2 O 4 -like species forms upon Al modification and converts further to CuAlO 2 -like species during aging, while the accumulation of CuO-like species is inhibited. The high affinity of Al-containing species ( i.e. , Al 2 O 3 and CuAl 2 O 4 -like species) with Cu(OH) 2 is suggested by DFT calculations, indicating that Cu(OH) 2 detached from ion-exchange sites are captured by Al to form CuAlO 2 -like species instead of CuO-like species. The passivation of detached Cu species by coated Al leads to somewhat weakened low-temperature SCR activity, but successfully preserves the high-temperature SCR performance upon aging, which can be applied to high-temperature SCR scenarios.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2021
·Vol. 29
·期 20
·29613-29623
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IF 4.223
Zhao Dianjia,Ye Wenkang,Cui Wenxuan
As eco-friendly adsorption material, hydroxyapatite (Ca 5 (PO 4 ) 3 OH, HA) has been extensively applied to the removal of heavy metal ions. However, separating and recovering of HA powder after the adsorption process limits their application. Alginate-based composite beads (HCA) encapsulated with HA and cellulose were designed to remove Cu(II) from aqueous solution. Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS) were used for characteristic analysis. An extensive discussion in terms of HCA adsorption capacity, effect of various Cu(II) concentration, and analysis of the involved mechanisms of Cu(II) removal on the biosorption. HCA beads showed that the maximum adsorption capacity for Cu(II) of 64.14 mg/g at pH = 5 with 8 h contact time. The Langmuir adsorption isotherm and second-order kinetic model gave the closest fit. HCA beads display good regeneration ability after four cycles and offer potentiality for practical application.
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Materials Today Communications
·
2021
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IF 3.383
Yanqing Xue,Bo Li,Xinliang Wang,Xinlei Li,Han Zhang,Qitang Hao
Agglomeration behavior of TiB 2 particles in 5%TiB 2 /Al-4.5%Cu composites (all compositions are in wt.% unless otherwise specified) is studied by adding different content of Mg to improve its strength and ductility, a widely used in-situ molten salt reaction process is used to produce the composites. The results show that addition of Mg could not only significantly segregate TiB 2 particles but also further refine the α-Al grains and then improve the mechanical properties of the composites on the basis of TiB 2 particles. Here, 0.5% Mg is considered the optimum mass fraction for dispersion, refinement, and modification of particles based on the results of investigation. The yield strength (YS), ultimate tensile strength (UTS), elastic Young’s modulus (EM), and Vicker’s hardness (VHN) of the composites in T6 heat treatment are increased to 375 MPa, 486 MPa, 88 GPa, and 167 HV - an improvement of 21.8%, 16.5%, 20.9%, and 9.4%, respectively, versus the original TiB 2 /Al-4.5%Cu composite (308 MPa, 417 MPa, 63 GPa, and 153 HV). The elongation of the composite is improved by 20.9%. These merits are mainly attributed to addition of Mg, which increases the surface-spread coefficient of TiB 2 particles by reducing the surface tension of the Al melt, thereby improving the wettability .
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MATERIALS & DESIGN
·
2021
·
IF 7.991
Tayiba Ilyas,Fazal Raziq,Sharafat Ali,Amir Zada,Nasir Ilyas,Rahim Shaha,Yong Wang,Liang Qiao
Water splitting and CO 2 conversion are emerging energy transfer techniques to generate hydrogen and low carbon fuel as eco-friendly energy sources. Herein, a frugal and facile approach is reported for decorating MoS 2 nanosheets on copper nanorods to design MoS 2 /Cu architecture as a trifunctional catalyst for electrochemical water splitting and photocatalytic CO 2 conversion. Under optimized conditions, MoS 2 /Cu electrocatalyst shows high performance at an overpotential of 252 mV for oxygen evolution reaction and 160 mV for hydrogen evolution reaction to attain 20 mAcm −2 and 10 mAcm −2 current densities in alkaline medium. The improved efficiency is mainly credited to the synergistic effect of MoS 2 nanosheets and Cu nanorods architecture. The electrode delivered a cell voltage of ~1.508 V to impart about 10 mAcm −2 current density with high durability. Also, the negligible overpotential decay after running the cell for 12 h with 3000/HER and 2000/OER CV cycles suggests remarkable stability that makes it a promising electrocatalyst for energy production. The photocatalytic CO 2 conversion activity was also measured, where MoS 2 /Cu exhibited a significant efficiency of CO 2 to methane conversion (CH 4 ~ 23 µmol g −1 h −1 ). Based on the obtained results, it is foreseeable that this work validates the significance of transition metals tuning for electrocatalysts and photocatalysts toward more efficient water electrolysis and CO 2 reduction for potential large-scale energy applications.
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JOURNAL OF ELECTRONIC MATERIALS
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2021
·Vol. 50
·期 6
·3222-3227
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IF 1.938
Han Wensong,Guo Qin,Su Tianhui
Cu@HBP-SH@Ag particles have been prepared by a facile synthesis strategy. Initially, thiol-terminated hyperbranched polymer (HBP-SH) was synthesized by stepwise polymerization. Subsequently, Cu particles covered with HBP-SH were prepared by reduction technology using HBP-SH as dispersant and template. Finally, Cu@HBP-SH@Ag particles were obtained by reduction reaction. Fourier-transform infrared (FT-IR) and ultraviolet–visible (UV–Vis) spectroscopy confirmed presence of HBP-SH on the surface of the Cu particles. The crystal structure was examined by x-ray diffraction (XRD) analysis. Scanning electron microscopy (SEM) and energy-dispersive spectrometry (EDS) analysis confirmed formation of Cu@HBP-SH@Ag particles. Thermogravimetric analysis (TGA) showed that the Cu@HBP-SH@Ag particles had better antioxidation properties than the Cu particles.
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ACS Catalysis
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2021
·
IF 13.084
Hong Li,Tian-Wen Jiang,Xianxian Qin,Jie Chen,Xian-Yin Ma,Kun Jiang,Xia-Guang Zhang,Wen-Bin Cai
Electrochemical CO2 reduction reaction (CO2RR) on Cu is often plagued by low selectivity and stability because of less-controlled preparation of electrocatalytic materials as well as insufficient understanding of the structure–performance relation. In this work, we develop a facile galvanic displacement protocol, involving an electropolished Cu sheet in a mixed Sb(III)–Cl– precursor solution, to form an Sb-modified Cu electrode that can selectively convert CO2 to CO with a Faradaic efficiency of ca. 82% and an undecayed reduction current over 12 h. Moreover, in situ infrared spectroscopy detects a relatively weak and red-shifted CO band on the Sb-modified Cu electrode as compared to that on the Cu electrode at potentials of CO2RR. Density functional theory calculations reveal that the Sb clusters on the Cu surface change the electronic structures of Cu as well as Sb and thus weaken the CO binding strength on Cu sites, consistent with the observed CO band feature and high CO selectivity. These findings may shed light on the rational design of high-selectivity CO2RR electrocatalysts by proper interfacial structure engineering.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2021
·Vol. 96
·期 8
·2382-2389
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IF 3.174
Jianxin Tang,Jianmin Huang,Thein Tun,Sihua Liu,Jue Hu,Guiyin Zhou
BACKGROUND At present, various kinds of hydrogel adsorbents are applied to the treatment of heavy metal ions in wastewater. In this work, we focused on the adsorption of cadmium [Cd(II)] and copper [Cu(II)] onto microspheres of a novel thermosensitive hydrogel (NH 2 -SA/PNIPA, aminated sodium alginate/poly- N -isopropyl acrylamide), studied the effect of temperature on the phase transition of the hydrogel in detail, and discussed the influence on the adsorption behavior of metal ions in the hydrogel. RESULTS The NH 2 -SA/PNIPA exhibited a higher adsorption efficiency under the conditions of interfering monovalent cationic and neutral pH. The adsorption capacities based on the Langmuir model were 57.2 mg g –1 for Cu(II) and 100.5 mg g –1 for Cd(II) at 20 °C, respectively. Higher temperature facilitated the adsorption process and also led to the volume shrinkage and hydrophobicity of NH 2 -SA/PNIPA. The metal ions had different hydration and hence different adsorption capacities, of 56.7 mg g –1 for Cu(II) and 88.6 mg g –1 for Cd(II) at 40 °C. The results of diffusion behavior analysis showed that the diffusion coefficients were ≈1 × 10 −11 m 2 s –1 . The adsorption performance of NH 2 -SA/PNIPA hardly decreased even after five cycles. In addition, the adsorption process was controlled mainly by the complexation reaction. CONCLUSION The novel hydrogel microspheres overcame the deficiency of conventional adsorbents and possessed high diffusibility. This work provides a theoretical basis and empirical evidence for enhancement of adsorbents for removing heavy metals in wastewater. © 2021 Society of Chemical Industry (SCI).
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Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Zhifei Hao,Guoquan Liu,Nan Ma,He Zhang,Yi Li,Yuguo Xia,Dongpeng Zhang,Sihui Zhan
Acidity and redox properties of the catalyst are two crucial factors affecting the performance of NH 3 -SCR. Herein, we design a novel WO x /Cu-CeO 2 oxide catalyst in which the WO x species are highly dispersed on the {111}/{100}-terminated surface of Cu-doped CeO 2 nanospheres , which exhibits great deNO x activity advantage and wide operating temperature window (200–400 °C, over 85% NO x conversion with a gas hourly space velocity (GHSV) of 60,000 h −1 ), as well as good sulfur resistance and N 2 selectivity . The relationship among the composition, acidity and redox properties of the WO x /Cu-CeO 2 catalyst is established in the NH 3 -SCR reaction. The combined experimental studies and spectroscopic characterization reveal that the introduction of Cu into the lattice of CeO 2 not only increases the surface Ce 3+ and oxygen vacancy concentration but also provides more sites for capture and dispersion of WO x species, thus mediating and improving the Lewis and Brønsted acid sites and reducibility of catalyst. XPS and DFT calculations further demonstrate that electronic interaction between WO x and Cu-doped CeO 2 is enhanced duo to the existence of interactions of short-range Ce-O-Cu and Ce-O-W. Moreover, the NH 3 -SCR reaction over WO x /Cu-CeO 2 may follow both Langmuir-Hinshelwood and Eley-Rideal reaction pathway according to the in situ DRIFTS.
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Journal of Materials Chemistry A
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2021
·Vol. 9
·期 13
·8372-8377
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IF 12.732
Songliang Liu,You Xu,Shiqian Jiao,Wenjing Tian,Tongqing Zhou,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
Current methods for industrial-scale ammonia synthesis rely excessively on fossil fuels, causing severe CO2 emissions. The electrochemical nitrogen reduction reaction (NRR) is a sustainable and environmentally friendly technology for ammonia synthesis under environmental conditions. Herein, we demonstrate the rational construction of Au3Cu@Cu nanocages with unique porous core–shell heterostructured walls by a facile two-step synthetic strategy. Due to the hollow cavities, porous core–shell heterostructured walls, and Au3Cu@Cu two-component composition, the as-constructed Au3Cu@Cu nanocages exhibit excellent NRR performance in 0.1 M Na2SO4 saturated with N2, achieving a high ammonia yield up to 33.97 μg h−1 mgcat.−1 and a faradaic efficiency of 21.41% at −0.2 V (vs. the reversible hydrogen electrode). This study will provide insight into the reasonable design and construction of hollow nanostructures with porous heterostructured walls for electrocatalytic applications.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Wenxin Liu,Zhaofan Tao,Duo Wang,Qianqian Liu,Yinan Zhang,Yanling Zhang,Alideertu Dong
The past several decades have witnessed tremendous research to discover ways for controlling heavy metal pollution, but most of the strategies do not involve reuse of the captured heavy metals. Herein, we propose a graphene oxide -based strategy for the effective removal of Cu 2+ ions from water, coupled with their reuse as an antibacterial agent. Using GO nanosheets as an adsorbent and nanosupport, the Cu 2+ ions were effectively extracted from water (>99.9%) and reduced in situ to copper nanoparticles (Cu NPs) containing both crystalline Cu and Cu 2 O. The as-captured Cu NPs showed efficient in vitro antibacterial ability against Escherichia coli , reducing the bacteria from 10 9 to 10 1 CFU mL –1 by using 1 mg mL –1 Cu NPs/GO NSs for 1 h. The minimum inhibitory concentration determined to be only 16 μg mL –1 . For practical applications, Cu recovered from wastewater could reduce bacteria by 8 log CFU in 1 h. The recovered Cu was still able to reduce the bacteria by 7 log CFU after 2 months of storage in an argon atmosphere. This strategy of extracting heavy metals and subsequently reutilizing to kill bacteria will be of great significance for environmental remediation and public healthcare.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Lele Cui,Zhiwen Li,Qingqing Li,Meifei Chen,Wenheng Jing,Xuehong Gu
The development of transition metal oxide-based integrated carbonaceous materials for use as bifunctional electrodes of high stability and activity in the heterogeneous electro-Fenton (EF) process is supposed to have great potential in environmental governance. Herein, Cu/CuFe 2 O 4 (CCFO) with different Cu 0 ratios were synthesized by a facile one-step solvothermal approach. These materials were subsequently used to fabricate modified graphite felt through the polytetrafluoroethylene (PTFE)-bonding technique. Importantly, with its hydrophobicity PTFE effectively inhibited metal leaching from the thus obtained cathodes and improved the oxygen utilization rate. Cathode performance in EF-based tetracycline (TC) degradation was found to increase with Cu 0 ratio. The observed increase in activity was attributed to Cu 0 enhancing the 2-electron oxygen reduction reaction selectivity (i.e., H 2 O 2 production) and endowing the cathode with abundant electron-rich centers that accelerated active Fe(II) regeneration, causing rapid conversion of H 2 O 2 to hydroxyl radical ( OH). The possible TC mineralization pathway was inferred by liquid chromatography–mass spectrometry (LC–MS) analysis, and a catalytic mechanism of the heterogeneous EF process was proposed. The most effective cathode fabricated displayed high stability even at pH 3 (0.84 ± 0.11 mg/L Fe and 1.35 ± 0.17 mg/L Cu leaching) and exhibited nearly 80% TC removal efficiency after five oxidation cycles, demonstrating its potential use in heterogeneous EF technology for efficient and durable wastewater treatment.
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NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 42
·18173-18184
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IF 3.288
Yi-Hu Ke,Xue Wang,Hong-Yu Qin,Hai Liu,Hong Yuan,Chun-Ling Liu,Wen-Sheng Dong
A series of Au catalysts supported on Cu–Al composite oxides were prepared and applied for the selective catalytic oxidation of glycerol to 1,3-dihydroxyacetone (DHA) in base-free conditions. The optimal Au/CuAlO-3 catalyst (the molar ratio of Cu/Al was 5 : 1) exhibited the best performance, and reached the glycerol conditions of 76.7% and DHA selectivity of 97.3% under the optimized reaction conditions. The high catalytic activity of the Au/CuAlO-3 catalyst correlated to the large concentration of surface-active oxygen species, the low reduction temperature of the support, the small size of Au nanoparticles (NPs) and the interactions between Au NPs and the support. This work demonstrates that Cu–Al composite oxides are promising supports for selective catalytic oxidation of glycerol to DHA, and may offer guidelines for designing efficient support for the selective conversion of glycerol to other high value-added products.
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