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Open Chemistry · 2020 ·Vol. 18 ·期 1 ·97-107 · IF 1.216

Amino-functionalized graphene oxide for Cr(VI), Cu(II), Pb(II) and Cd(II) removal from industrial wastewater

Huayu Huang,Yang Wang,Yubin Zhang,Zhiying Niu,Xinli Li

Amino-functionalized graphene oxide (GO-NH 2 ) was synthesized by grafting (3-aminopropyl) triethoxysilane on the graphene oxide (GO) surface. The GO-NH 2 with high surface area and numerous active sites can efficiently adsorb Cr(VI), Cu(II), Pb(II) and Cd(II) ions. The maximum adsorption capacities of GO-NH 2 for Cr(VI), Cu(II), Pb(II) and Cd(II) were 280.11, 26.25, 71.89 and 10.04 mg g −1 , respectively. The pseudo-first-order and pseudo-second-order kinetic models were employed to describe the kinetic processes. The experimental data agreed well with the pseudo-second-order kinetic equation, and the adsorption of heavy metals onto GO-NH 2 occurs via chemical adsorption. The characteristics of Cr(VI), Cu(II), Pb(II) and Cd(II) in the GO-NH 2 adsorption processes were analyzed using the Langmuir and Freundlich isotherm models. The adsorption processes of Pb(II) and Cd(II) on GO-NH 2 were fit by the Langmuir model. The Freundlich isotherm model was well correlated to Cr(VI) and Cu(II). The GO-NH 2 is a promising material for the removal of heavy metal ions from industrial wastewater. This study provides an effective pathway to process industrial wastewater, and the GO-NH 2 has a good adsorption effect for the treatment of heavy metals in industrial wastewater.

研究领域: 环境科学 · 化学工程 · 材料科学 · 水处理
✓ 已验证 DOI 高影响因子
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2022 · IF 10.319

Uncover the mystery of interfacial interactions in immiscible composites by spectroscopic microscopy: A case study with W-Cu

Zhi Zhao,Fawei Tang,Chao Hou,Xintao Huang,Xiaoyan Song

Characterizing immiscible metallic composites with electron microscopy and X-ray spectroscopy is the classic way of obtaining their structural and physical details. Nevertheless, such a combination lacks ability to tell the interfacial interactions at grain boundaries. Here we demonstrate a novel strategy to uncover the mystery of interfacial interactions in such systems by spectroscopic microscopy. The morphological and spectral data of samples were simultaneously recorded and analyzed, which reveals critical information regarding interfacial electronic modes. Taking W-Cu as a model, we experimentally quantified its connectivity and unambiguously identified conditional bonding between W and Cu. Further, we chemically reconstructed the specific W-Cu boundary that possessed the strongest interactions and investigated its atomic structure. The mechanism of W-Cu bonding was proposed and verified by first-principle calculations. The above methodology holds great promise to serve as a universal approach in achieving in-depth understanding of immiscible composites.

研究领域: 材料科学 · 冶金学 · 显微镜技术 · 光谱学
✓ 已验证 DOI 高影响因子
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JOURNAL OF ENVIRONMENTAL ENGINEERING · 2020 ·Vol. 147 ·期 1 ·04020142 · IF 1.264

Efficient Adsorption of Tetracycline Using Cu+-Modified SBA-15 and Its Adsorption Mechanism

Yuefeng Qiu,Liming Kong,Tonghe Chen,Qin Xu

Cu+-modified SBA-15 (Cu+/SBA-15, SBA-15 refers well-ordered hexagonal mesoporous silica) was prepared for adsorption of tetracycline (TC) by the pH adjusting reduction method. Some Cu+ species (Cu2O) are aggregated on the outside surface of SBA-15, and the other Cu+ species are highly dispersed in SBA-15 via ≡Si-O-Cu. Its adsorption mechanism was firstly studied via comparison with CuO/SBA-15. The TC adsorption kinetic of Cu+/SBA-15 fitted the pseudo-second-order model well. The adsorption isotherms at 293, 303, and 313 K were determined and modeled with Langmuir and Freundlich equations, and the Qmax of Cu+/SBA-15 for TC calculated from Langmuir model could reach 961.54  mg/g at 313 K. Its good adsorption performance for TC is associated with the high surface area of SBA-15, highly dispersed Cu+ species, and mesoporous structure. The adsorption of Cu+/SBA-15 for TC is an endothermic process, and adsorption heat is 66.88  kJ·mol−1, which implies that the adsorption process of Cu+/SBA-15 for TC is weak chemisorption. The adsorption mechanism of Cu+/SBA-15 was mainly explored via comparing with CuO/SBA-15 by Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) spectroscopy analysis. Besides the coordination complexation of Cu+ with NH2 radical of TC, the π-complexation between Cu+, and the benzene ring of TC improved the adsorption capacity of Cu+/SBA-15 for TC comparing with CuO/SBA-15 and showed a dominant role for TC adsorption.

研究领域: 环境科学 · 材料科学 · 化学工程 · 分析化学
✓ 已验证 DOI 高影响因子
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Journal of Macromolecular Science Part A-Pure and Applied Chemistry · 2019 · IF 1.163

Removal of Cd(II) and Cu(II) ions from aqueous solutions using tannin-phenolic polymer immobilized on cellulose

Peng Zhou,Hua Yuan,Lijun Ou,Peng Zhiyuan

Tannin was crosslinked with paraformaldehyde to prepare tannin-phenolic polymer(TP), TP immobilized on cellulose (TPPC) was prepared by the cross-linking reaction of TP and cellulose with epichlorohydrin as crosslinking agent. Tannin was crosslinked prior to being immobilized on cellulose, which could increase the effective phenolic hydroxyl content in cellulose skeleton and improve the adsorption property of TPPC for metal ions. The maximum adsorption capacity of TPPC for Cd(II) and Cu(II) ions were 80.11 mg/g and 55.97 mg/g, respectively. The adsorption equilibrium data for the metal solutions fitted the Langmuir model well. The adsorption rate data fitted well to a Pseudo-second-order model. The TPPC has potential application value in the field of metal wastewater treatment.

研究领域: 环境科学 · 高分子科学 · 水处理技术 · 吸附技术 · 化学工程
✓ 已验证 DOI 高影响因子
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Journal of Materials Chemistry A · 2021 ·Vol. 9 ·期 40 ·23234-23242 · IF 12.732

Facile synthesis of an antimony-doped Cu/Cu2O catalyst with robust CO production in a broad range of potentials for CO2 electrochemical reduction

Hongyu Chen,Zhaojie Wang,Shoufu Cao,Siyuan Liu,Xiaojing Lin,Yi Zhang,Yizhu Shang,Qiuying Zhu,Sainan Zhou,Shuxian Wei,Baojun Wei,Daofeng Sun,Xiaoqing Lu

The electrocatalytic CO2 reduction reaction (CO2RR) on copper-based catalysts is a promising method to produce valuable chemicals, but its selectivity is much lower than expected largely due to insufficient research on the structure of new materials. Herein, the antimony-doped Cu/Cu2O (Cu/Cu2O–Sb) catalyst is developed for a highly selective CO2RR to CO. The synthesized Cu/Cu2O–Sb exhibits intensive suppression of hydrogen evolution, a low overpotential and high faradaic efficiency (FE) towards CO. The CO selectivity is as high as ∼95% with a partial current density of ∼6.3 mA cm−2 at −0.9 V and maintains over 90% in a broad range of potentials. DFT calculations reveal that the doping of antimony achieves the distinct activation of CO2 and suppression of hydrogen evolution. Meanwhile, the pre-adsorbed *CO significantly promotes the desorption of the neighboring *CO, which is the key for high selectivity of CO2RR to CO. This work will provide a new consideration for the origin of high selectivity during the CO2RR and pave the way toward design of highly selective CO2 reduction catalysts.

研究领域: 电化学 · 催化 · 材料科学
✓ 已验证 DOI 高影响因子
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Small · 2024 · IF 13

Activating Redox Kinetics of Li2S via Cu+, I− Co-Doping Toward High-Performance All-Solid-State Lithium Sulfide-Based Batteries

Jing Gao,Yuan Gao,Jinghua Hao,Xiaolin Sun,Fuhua Zhao,Yuan Zhang,Wenyan Si,Jianfei Wu

All-solid-state lithium sulfide-based batteries (ASSLSBs) have drawn much attention due to their intrinsic safety and excellent performance in overcoming the polysulfide shuttle effect. However, the sluggish kinetics of Li 2 S cathode severely impede commercial utilization. Here, a Cu + , I − co-doping strategy is employed to activate the kinetics of Li 2 S to construct high-performance ASSLSBs. The electronic conductivity and Li-ion diffusion coefficient of the co-doped Li 2 S are increased by five and two orders of magnitude, respectively. Cu + as a redox medium greatly improves the reaction kinetics, which is supported by ex situ X-ray photoelectron spectroscopy. Density functional theory calculation (DFT) shows that Cu + , I − co-doping reduces the Li-ions diffusion energy barrier. The co-doped Li 2 S exhibits a remarkable improvement in capacity (1165.23 mAh g −1 (6.65 times that of pristine Li 2 S) at 0.02 C and 592.75 mAh g −1 at 2 C), and excellent cycling stability (84.58% capacity retention after 6200 cycles at 2 C) at room temperature. Moreover, an ASSLSB, fabricated with a lithium-free (Si─C) anode, obtains a high specific capacity of 1082.7 mAh g −1 at 0.05 C and 97% capacity retention after 400 cycles at 0.5 C. This work provides a broad prospect for the development of ASSLSBs with practical energy density exceeding that of traditional lithium-ion batteries.

研究领域: 材料科学 · 电化学 · 电池技术
✓ 已验证 DOI 高影响因子
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

Study on the influence of Cu/F dual-doping on the Fe–Mn based compound as cathode material for sodium ion batteries

Yixuan Zhang,Guoqiang Liu,Chang Su,Guangyin Liu,Hongda Sun,Danlei Qiao,Lei Wen

This work focuses on the improvement on the electrochemical performances of Fe–Mn based oxides as cathode for sodium ion batteries by doping Cu and F elements. The synthesized doped-compounds exhibit extremely excellent electrochemical performance. For instance, it's initial discharge capacity can reach 195.6 mAh g −1 at a current density of 10 mA g −1 . Meanwhile, after 200 cycles at 200 mA g −1 , it still remains a capacity of 124.1 mAh g −1 , 87.8% of the initial capacity of 141.3 mAh g −1 . More significantly, it can deliver a high capacity of 106.4 mAh g −1 at a high current density of 1000 mA g −1 . It is found that F/Cu co-substitution obviously improve the discharge capacity and cycle stability of Fe–Mn based oxide especially at higher current densities. Doping Cu and F elements has influence on the structure and morphology of the material, which results in the improvement of charge-discharge characteristics.

研究领域: 材料科学 · 电化学 · 能源存储
✓ 已验证 DOI 高影响因子
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AICHE JOURNAL · 2019 ·Vol. 66 ·期 1 ·e16746 · IF 3.463

Mechanistic and kinetic investigation of Cu(II)-catalyzed controlled radical polymerization enabled by ultrasound irradiation

Chao Bian,Yin-Ning Zhou,Zheng-Hong Luo

Controlled radical polymerization (CRP) under external field has been an attractive research area in these years. In this work, a new electron transfer mechanism, that is, sonochemically induced electron transfer (SET) was introduced to mediate polymerization for the first time. The activator Cu I X/L complex was (re)generated from Cu II X 2 /L in dimethylsulfoxide (DMSO) by the SET process in the presence of free ligand tris(2-dimethylaminoethyl)amine (Me 6 TREN). The investigation of polymerization including the mechanistic insights and effect of experimental conditions on the rate of reaction has been undertaken. Kinetics of Cu(II)-catalyzed CRPs via SET under different conditions (i.e., Me 6 TREN concentration, catalyst loading, targeted degree of polymerization, and sonication power) were conducted in an unprecedentedly controlled manner, yielding polymers with predetermined molar masses and low dispersities ( Đ < 1.12). Attractively, the polymerization can be performed without the piezoelectric nanoparticles and exogenous reducing agent. Contamination by nonliving chains formed from sonochemically generated radicals is avoided as well. All of these results supported that Cu(II)-based catalyst activation enabled by ultrasonication has a promising potential in scale-up of CRP.

研究领域: 高分子化学 · 材料科学 · 化学工程
✓ 已验证 DOI 高影响因子
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Nano Research · 2023 ·Vol. 17 ·期 5 ·4437-4443 · IF 9.9

Neutral color and self-healable electrochromic system based on CuI/Cu and $${{\rm{I}}_3}^ - /{{\rm{I}}^ - }$$ conversions

Zhong Junsen,Huang Bingkun,Yang Kunjie,Ma Zuju,Du Lingyu,Luo Ning,Tang Fengjiao,Hou Chuanxin,Jiang Fuyi,Kang Litao

The electrochromic (EC) mechanisms of inorganic materials are usually based on reversible cation insertion/extraction or metal deposition/dissolution, which are plagued by ion trapping and dendrite growth, respectively. In this paper, a novel conversion-type electrochromic mechanism is proposed, by making good use of the CuI/Cu redox couple. This CuI-based electrochromic system shows a neutral color switching from transparent and dim grey. By simply increasing the bleaching voltage, \({{\rm{I}}_3}^ - /{{\rm{I}}^ - }\) redox couple can be further activated. The generated \({{\rm{I}}_3}^ - \) will readily react with Cu, effectively improving the conversion reversibility and thereby rejuvenating the degraded electrochromic performance. Thanks to the well-designed electrode and the self-healing ability, this conversion electrochromic system achieves rapid response times ( t coloring : 23 s, t bleaching : 6 s), decant optical modulation amplitude (26.4%), high coloration efficiency (86.15 cm 2 ·C −1 ), admirable cyclic durability (without performance degradation after 480 cycles) and excellent optical memory ability (transmittance variation < 1% after 10 h open-circuit storage). The establishment of this conversion-type electrochromism may inspire the exploration of novel electrochromic materials and devices.

研究领域: 材料科学 · 电化学 · 纳米技术 · 智能材料 · 能量存储与转换
✓ 已验证 DOI 高影响因子
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Polymer Chemistry · 2021 ·Vol. 12 ·期 30 ·4347-4358 · IF 5.582

Cu-Catalyzed four-component polymerization of alkynes, sulfonyl azides, nucleophiles and electrophiles

Junnan He,Nan Zheng,Ming Li,YuBin Zheng,Wangze Song

Multicomponent polymerization has emerged as a promising strategy to develop functional polymers with versatile structures. In this work, a Cu-catalyzed four-component polymerization was developed using diynes, sulfonyl azides, nucleophiles, and a variety of electrophiles including alkyl glyoxylates, nitroalkenes, and Morita–Baylis–Hillman adducts to successfully synthesize a library of α-functionalized poly(N-sulfonylimidates)s with a wide substrate scope and high molecular weights (up to 20 000 g mol−1) in high yields (up to 86%). Such α-functionalized poly(N-sulfonylimidates)s could be further post-modified or utilized for the design of multi-functional and biodegradable polymers.

研究领域: 高分子化学 · 材料科学
✓ 已验证 DOI 高影响因子
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Journal of Materials Chemistry A · 2023 ·Vol. 12 ·期 2 ·1218-1232 · IF 11.9

SiO2 assisted Cu0–Cu+–NH2 composite interfaces for efficient CO2 electroreduction to C2+ products

Zi-Yang Zhang,Hao Tian,Han Jiao,Xin Wang,Lei Bian,Yuan Liu,Nithima Khaorapapong,Yusuke Yamauchi,Zhong-Li Wang

The electrochemical CO2 reduction reaction (CO2RR) for high value-added multi-carbon product (C2+) production over copper oxide-based catalysts is an important way to realize the carbon cycle. However, developing effective reaction interfaces and microenvironments to improve the Faraday efficiency (FE) and current density of C2+ remains a major challenge. Herein, we construct Cu0–Cu+–NH2 composite interfaces with the assistance of SiO2. Using Cu2O nanoparticles as a model catalyst, a layer of porous SiO2 is first coated on the surface of the particles, and then, a silane coupling agent containing –NH2 is bonded on the surface of SiO2. The strong interaction between SiO2 and Cu2O at the interface induces the oxidation effect of low valent Cu, and even under the CO2RR, part of Cu+ is reduced to Cu0 and part of Cu+ still maintains positive valence, forming the interface of Cu0–Cu+. SiO2 also acts as a bridge between copper species and –NH2 to create a Cu catalyst–NH2 group interface. With the help of the synergistic effect of the composite interfaces, the optimized Cu2O@SiO2–NH2 catalyst achieves a FE of 81.2% for C2+ products with a current density of 292 mA cm−2 at −1.7 V versus a reversible hydrogen electrode. In situ Raman and attenuate total reflectance-infrared absorption spectroscopy spectra show that the interaction between surface –NH2 and CO2 molecules enhances the adsorption and activation process of CO2 and promotes the formation of CO intermediates (*CO). On the Cu0–Cu+ interface, the C–C coupling process between *CO is accelerated, and the two interfaces synergistically promote the generation of C2+ products. This work provides a new strategy for constructing composite interfaces to improve the CO2RR to C2+ products.

研究领域: 电化学 · 材料科学 · 催化 · 可持续能源
✓ 已验证 DOI 高影响因子
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Catalysis Science & Technology · 2024 · IF 4.4

Study on graphitic carbon nitride catalysts with Bi and Cu loaded for carbon dioxide photothermal reduction

Bin Guan,Junyan Chen,Zhongqi Zhuang,Lei Zhu,Zeren Ma,Xuehan Hu,Chenyu Zhu,Sikai Zhao,Kaiyou Shu,Hongtao Dang,Zhen Huang

As a significant technology of CO2 utilization, artificial CO2 photoreduction has received more and more attention. Herein, g-C3N4 catalysts modified with Bi and/or Cu for CO2 photothermal reduction were prepared by solvothermal synthesis and impregnation methods. Performance evaluation and physicochemical and photo- and thermochemical characterization indicated that Bi and Cu modification effectively enhanced the photo-absorption properties of g-C3N4 catalysts, improving charge transfer efficiency and catalytic performance. Compared with single-metal modification, Bi and Cu co-modification showed a narrower bandgap and more excellent light and CO2 absorption capacity, suggesting a certain synergistic effect of Bi and Cu co-modification. The alteration of the light absorption properties may be related to the surface plasmon effect of Bi and Cu, and the co-loading of Bi and Cu can exacerbate the effect, which can effectively enhance the photoresponsivity of the catalysts, leading to higher catalytic performance.

研究领域: 催化 · 材料科学 · 环境科学 · 化学工程
✓ 已验证 DOI 高影响因子
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