ACS Nano
·
2023
·
IF 17.1
Yanfei Sun,Jiangzhou Xie,Zhenzhen Fu,Huiying Zhang,Yebo Yao,Yixiang Zhou,Xiaoxuan Wang,Shiyu Wang,Xueying Gao,Zheng Tang,Shuyuan Li,Xiaojun Wang,Kaiqi Nie,Zhiyu Yang,Yi-Ming Yan
Efficient conversion of carbon dioxide (CO2) into value-added materials and feedstocks, powered by renewable electricity, presents a promising strategy to reduce greenhouse gas emissions and close the anthropogenic carbon loop. Recently, there has been intense interest in Cu2O-based catalysts for the CO2 reduction reaction (CO2RR), owing to their capabilities in enhancing C–C coupling. However, the electrochemical instability of Cu+ in Cu2O leads to its inevitable reduction to Cu0, resulting in poor selectivity for C2+ products. Herein, we propose an unconventional and feasible strategy for stabilizing Cu+ through the construction of a Ce4+ 4f–O 2p–Cu+ 3d network structure in Ce-Cu2O. Experimental results and theoretical calculations confirm that the unconventional orbital hybridization near Ef based on the high-order Ce4+ 4f and 2p can more effectively inhibit the leaching of lattice oxygen, thereby stabilizing Cu+ in Ce-Cu2O, compared with traditional d–p hybridization. Compared to pure Cu2O, the Ce-Cu2O catalyst increased the ratio of C2H4/CO by 1.69-fold during the CO2RR at −1.3 V. Furthermore, in situ and ex situ spectroscopic techniques were utilized to track the oxidation valency of copper under CO2RR conditions with time resolution, identifying the well-maintained Cu+ species in the Ce-Cu2O catalyst. This work not only presents an avenue to CO2RR catalyst design involving the high-order 4f and 2p orbital hybridization but also provides deep insights into the metal-oxidation-state-dependent selectivity of catalysts.
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Nanotechnology Reviews
·
2023
·Vol. 12
·期 1
·
IF 7.4
Ke Chen,Xudong Yang,Rui Hao,Minghui Shao,Xiaoyong Yang,Xiuze Li,Yuxuan Li,Juzhe Liu,Sai Zhang
Activation of peroxymonosulfate (PMS) to degrade persistent organic contaminants has received increasing attention in wastewater purification. In this study, Cu 2 O catalysts with different exposed crystal facets were prepared, characterized, and evaluated for acetaminophen (ACE) degradation through PMS activation. The experimental results showed that cubic Cu 2 O with {100} facets exhibited remarkable activity on ACE removal by PMS activation in wide pH range of 3–11. DFT calculations indicated that Cu 2 O-{100} displayed higher electron transfer efficiency and PMS adsorption ability, further improving PMS activation. The radicals quenching experiments and electron paramagnetic resonance (EPR) results illustrated that singlet oxygen ( 1 O 2 ) was dominant reactive oxidative species (ROSs) during oxidation reactions and the relevant generation pathways were distinctly elucidated. Finally, the possible PMS activation mechanisms were discussed for ACE degradation in a wide pH range. This study will provide new insights to disclose PMS-based advanced oxidation processes (AOPs), and offer a new approach for wastewater purification by non-radical reactions.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Baofang Zhang,Ziyu Zengcai,Wenting Lin,Meijin Zhang,Yunhong Pi,Tiejun Wang
Photothermal synergism can effectively activate methanol at low operating temperature and significantly reduce the activation energy of the reaction, achieving more efficiently H 2 release from methanol reforming. Here, a novel hierarchical heterojunction that integrating photo- and thermal-active Cu 2 O catalytic species with in-situ derived NH 2 -MIL-125@TiO 2 framework was specifically designed for photothermal-driven aqueous phase reforming of methanol into H 2 . The afforded Cu 2 O/NH 2 -MIL-125@TiO 2 realized an outstanding photothermal H 2 production activity (apparent quantum efficiency of 22.3 % at 365 nm), ca. 13-times higher than that of thermocatalytic condition. Interestingly, the photothermal effect did confer the Cu 2 O/NH 2 -MIL-125@TiO 2 with unexpected activity at low temperature subsided to 100 °C and accelerated the activation of MeOH/H 2 O with an obvious reduction of activation energy from 82.62 kJ·mol −1 to 52.40 kJ·mol −1 . The improvement of catalyst stability and the promotion of charge separation also contributed to a long-term photothermal H 2 evolution activity with average rate of 1.49x10 6 μmolg Cu -1 h −1 and a total turnover number (TON) up to 5971 in 63 h, almost 125-fold promotion compared with Cu 2 O.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2023
·
IF 10.9
Xiao Wang,Tongxin Di,Wei Li,Debao Liu,Xiaohao Sun
Nowadays, Zinc (Zn)-based biocomposites as biodegradable implant materials have been recognized as a promising approach to overcome the insufficient mechanical performance of Zn matrix and to endow the Zn-based materials with biofunctionality. However, the strengthening effect on Zn-based matrix composite remains far from expectation mainly due to the poor interfacial bonding between the reinforcement and Zn matrix, and the relatively coarse grain size of the Zn matrix. Herein, we have developed a novel in situ wetting strategy to ameliorate the interfacial bonding and mechanical performance of Zn-Ag-based composites using cuprous oxide-modified graphene oxide (Cu 2 O-GO) sheets as reinforcement. The enhanced interfacial bonding between GO sheets and Zn matrix owing to the in situ generated ZnO interlayer and the ultrafine microstructure with an average grain size of 360 nm were simultaneously achieved in the hot extruded (HEed) 1 wt%Cu 2 O-GO/Zn-2 wt%Ag biocomposites. Consequently, HEed biocomposites possessed excellent tensile properties, including ultimate tensile strength (UTS) of 344.0 ± 2.4 MPa, yield stress (YS) of 314.0 ± 4.8 MPa, and elongation at failure of 15.5% ± 1.3%. Ultrafine and uniform microstructure of the HEed biocomposites resulted in a relatively uniform corrosion morphology and a degradation rate of 0.195 ± 0.004 mm y −1 in simulated body fluid (SBF) solution. The 2-fold diluted extract of the HEed biocomposites exhibited satisfying cytocompatibility with MC3T3-E1 pre-osteoblast comparable to that of Ti-6Al-4 V ELI alloys. More importantly, the synergistic effect of metallic ions, Ag-rich nanoparticles, and GO sheets contributed to the remarkable antibacterial activity of the experimental biocomposites against both S. aureus and E. coli. These results demonstrated that the 1Cu 2 O-GO/Zn-2Ag biocomposites should be anticipated as a promising biodegradable material for orthopedic applications.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2018
·Vol. 317
·期 2
·959-968
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IF 1.181
Zhang Xiaoyuan,Gu Ping,Zhou Shishuai,Dong Lihua,Zhang Guanghui
A synthesis method was introduced for the large-scale preparation of a nano Cu 2 O/Cu-modified activated carbon composite, L-nano Cu 2 O/Cu–C. As the adsorbent, the synthesized composite could efficiently remove radioactive iodide ions (I − ) from simulated water. A lab-scale integrated novel countercurrent two-stage adsorption and membrane separator system was designed to assess the practical application of L-nano Cu 2 O/Cu–C. Stable and high I − removal efficiency was achieved during the operation of the system. The effluent met the water quality requirements, and the membrane fouling rate was lower. This study provides a potential process to treat water contaminated with radioactive I − in practical applications.
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MICROCHIMICA ACTA
·
2017
·Vol. 184
·期 11
·4331-4339
·
IF 4.58
Li Junhua,Jiang Jianbo,Xu Zhifeng,Liu Mengqin,Feng Haibo,Liu Youcai,Qian Dong
The authors report on a low temperature method for large-scale fabrication of cuprous oxide nanocubes deposited on nitrogen-doped reduced graphene oxide (Cu 2 O/N-RGO). The material was deposited in a glassy carbon electrode (GCE) where it is found to display enhanced electrocatalytic activity for oxidation of diethylstilbestrol (DES). The morphology and composition of Cu 2 O/N-RGO were characterized by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy and energy-dispersive spectroscopy. The results demonstrate that the RGO is doped with 3.5% of nitrogen (atomic ratio), and that nanostructured Cu 2 O particles with controlled cubical morphology and an average size of about 450 nm have been homogeneously deposited on the surface of N-RGO sheets. The oxidation peak of DES was recorded at 0.315 V (vs. saturated calomel electrode) using differential pulse voltammetry. Under the optimal conditions, the modified GCE displays a linear response in the 0.3 to 150 μM DES concentration range, and the limit of detection is 10 nM. The method was applied to the determination of DES in spiked milk, meat and urine samples and gave excellent selectivity, stability and reproducibility.
A nanocomposite consisting of Cu 2 O nanocubes/N-doped reduced graphene oxide (Cu 2 O/N-RGO) for the electrochemical determination of diethylstilbestrol (DES). The Cu 2 O/N-RGO modified electrode displays a linear response in the 0.3 to 150 μM DES concentration range. The method was applied to the determination of DES in spiked milk, meat and urine samples
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2017
·
IF 2.536
Huixiang Ouyang,Aihui Liang,Zhiliang Jiang
The stable Cu 2 O nanocubic (Cu 2 ONC) sol was prepared, based on graphene oxide (GO) catalysis of glucose-Fehling's reagent reaction, and its absorption and resonance Rayleigh scattering (RRS) spectra, transmission electron microscopy (TEM) and energy dispersive spectroscopy (EDS) were examined. Using the as-prepared Cu 2 ONC as RRS probe, and coupling with the neomycin sulfate (NEO) complex reaction , a new, simple, sensitive and selective RRS-energy transfer (RRS-ET) method was established for detection of neomycin sulfate, with a linear range of 1.4–112 μM and a detection limit of 0.4 μM. The method has been applied to the detection of neomycin sulfate in samples with satisfactory results.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Yaqun Han,Jingyuan Hu,Jie Ren,Shufen Zhang,Suli Wu
Introducing structured color-generating microstructures on leather instead of dyestuffs is expected to be an effective solution to achieve high-performance colorful leather without harmful effluent. Here, based on the disordered thin-layer Cu2O or ZnS microstructure, we obtained a series of colorful leathers with both sparkling brilliant structural colors and excellent color durability, using polyurethane and polyacrylate as linkers. The brilliant colors were generated by Mie resonance of ZnS or Cu2O nanospheres, while the polymer binders provided color stability and unique high gloss. The brilliant color has a unique sparkling effect under light, and the structural color can be adjusted by the sizes of the Cu2O or ZnS spheres. The colorful leather has superior rubbing fastness (4–5 grades) and superior light fastness (5–6 grades) to maintain color stability. Additionally, multiple color patterns and large-area colorful leather can also be produced, displaying great potential in the sustainable development of the leather industry.
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OPTICAL MATERIALS
·
2024
·
IF 3.8
Mengyao Xue,Jingwei Han,Xing Dai,Yucai Ge,Yunhua Zhang,Zibin Hai
Cu 2 O–SiC/g-C 3 N 4 composite photocatalysts with excellent photocatalytic performance under visible light were synthesized for the first time via a facile approach combining calcination with hydrothermal reaction. Comprehensive characterization of the synthesized samples encompassing composition, morphology, structure and photoelectric properties was conducted utilizing techniques such as X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), transmission electron microscopy (TEM), diffuse reflectance spectroscopy (DRS), photoluminescence spectroscopy (PL), and electrochemical impedance spectroscopy (EIS). Results unequivocally demonstrate successful preparation of the ternary composite through Cu 2 O loading onto SiC/g-C 3 N 4 , evincing markedly elevated activity compared to individual counterparts and binary composites. Notably, in the presence of the prepared Cu 2 O–SiC/g-C 3 N 4 , the degradation rate of methyl orange reached 93.70 % under illumination with a visible LED light rated at 5 W. The notable enhancement in photocatalytic performance of the ternary composites is primarily ascribed to the synergistic effects stemming from the formation of p-n junctions between Cu 2 O and g-C 3 N 4 , alongside the Z-scheme configuration established between Cu 2 O and SiC. Free radical quenching experiments corroborated •O 2 − and h + as the principal redox species mediating the visible light quenching process. This study not only presents a feasible strategy for the fabrication of Cu 2 O-based ternary composites with significantly augmented photocatalytic performance but also delineates a novel avenue for the design and construction of composite photocatalysts facilitating enhanced charge-carrier generation and separation concomitantly.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2016
·
IF 3.014
Jiayi Jin,He Mei,Huimin Wu,Shengfu Wang,Qinghua Xia,Yu Ding
The Cu 2 O@Pt nanoparticles were prepared by a two-step method, using Vulcan XC-72 carbon as support (donated as Cu 2 O@Pt/C). Transmission electron microscopy , X-ray diffraction and X-ray photoelectron spectroscopy were used to characterize the resulting Cu 2 O@Pt core-shell nanoparticles. The chemically modified electrode based on Cu 2 O@Pt/C nanocomposites was employed to eliminate the interference from ascorbic acid and uric acid for the sensitive and selective determination of dopamine. The electrochemical results indicate that the Cu 2 O@Pt/C nanocomposites show better electrocatalytic activity for the oxidation of dopamine than Pt/C nanocomposites with a linear range from 10 nM to 1027.16 μM, a detection limit of 3 nM (S/N = 3) and sensitivity of 638.0 μA mM −1 cm −2 . Moreover, the sensor exhibits excellent long-time stability, good reproducibility and can be applied for practical application.
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ELECTROCHIMICA ACTA
·
2015
·
IF 4.504
Yi-Tao Xu,Ying Guo,Le-Xin Song,Kai Zhang,Matthew M.F. Yuen,Jian-Bin Xu,Xian-Zhu Fu,Rong Sun,Ching-Ping Wong
Cuprous oxide (Cu 2 O) sub-microspheres @ reduced graphene oxide (rGO) nanosheets core-shell composites with 3D architecture are successfully fabricated by a one-step method through co-reduction of irregular cupric citrate and graphene oxide nanosheets at room temperature . Comparing to the bare Cu 2 O sub-microspheres and the simple physical mixture of Cu 2 O and rGO (Cu 2 O-rGO-M), the Cu 2 O@rGO electrodes demonstrate dramatically improved capacity, cyclic stability and rate capability as anode materials for lithium ion batteries . At a low current density of 100 mA∙g −1 , Cu 2 O@rGO electrodes deliver a discharge capacity of 534 mAh∙g −1 after 50 cycles, retaining 94% of the initial capacity. Under a higher current density of 1000 mA∙g −1 , Cu 2 O@rGO electrodes exhibit a discharge capacity of 181 mAh∙g −1 after 200 cycles, approximately 4 times larger than that of bare Cu 2 O sub-microsphere electrodes. The rate capacity retention of Cu 2 O@rGO electrode is 74% at 200 mA∙g −1 and 38% at 1000 mA∙g −1 relative to 100 mA∙g −1 , much better than that for Cu 2 O-rGO-M (52% and 34%) and bare Cu 2 O electrodes (13% and 3%,). The enhanced electrochemical performance for Cu 2 O@rGO might be ascribed to the rGO coating and 3D architecture. The outer coated rGO nanosheets could provide additional 3D conductive networks as well as serve as the buffer layers for accommodating the large volume change of the inner Cu 2 O sub-microspheres during the charge-discharge cycling.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Bo-hui Li,Kai-hua Zhang,Xiao-jing Wang,Yu-pei Li,Xinying Liu,Bao-Hang Han,Fa-tang Li
High-performance photocatalysts for catalytic reduction of CO 2 are largely impeded by inefficient charge separation and surface activity. Reasonable design and efficient collaboration of multiple active sites are important for attaining high reactivity and product selectivity . Herein, Cu-Cu 2 O and Ag nanoparticles are confined as dual sites for assisting CO 2 photoreduction to CH 4 on TiO 2 . The introduction of Cu-Cu 2 O leads to an all-solid-state Z-scheme heterostructure on the TiO 2 surface, which achieves efficient electron transfer to Cu 2 O and adsorption and activation of CO 2 . The confined nanometallic Ag further enhances the carrier’s separation efficiency, promoting the conversion of activated CO 2 molecules to •COOH and further conversion to CH 4 . Particularly, this strategy is highlighted on the TiO 2 system for a photocatalytic reduction reaction of CO 2 and H 2 O with a CH 4 generation rate of 62.5 μmol∙g −1 ∙h −1 and an impressive selectivity of 97.49 %. This work provides new insights into developing robust catalysts through the artful design of synergistic catalytic sites for efficient photocatalytic CO 2 conversion.
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