Journal of Cleaner Production
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2019
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IF 6.395
Yue Li,Huiqin Li,Shukun Le,Xue Bai,Xiaojing Wang
The conversion of the heavy concentration of nitroarenes into their corresponding non-toxic aminoarenes is very meaningful for both environment and industrial applications. In this study, a series of Cu 2 O/SrTiO 3 nanocomposites and further Cu 2 O/Cu/SrTiO 3 via Cu + reducing in situ during the reactive proceeding were fabricated and applied to reduce nitroarenes. The as-prepared composites present high reductive activity and reusable stability for 4-nitrophenol both under the continuous multi-batch ways and flow conditions. The test in an enlarged level revealed 4-nitrophenol (10 L, 0.01 mol L −1 ) could be quickly conversed to 4-aminophenol over the as prepared sample (300 mg) within 1 h under continuous flow conditions by a self-designed device. The mechanism investigation proposed that Cu 0 /Cu +1 pairs serve as a hydrogen and electron transferred shuttle to promote the reductive ability while SrTiO 3 as a protective agent packs up tetrakaidecahedron Cu 2 O to achieve a substantial increase in the stability of the catalyst. The existence of a Cu 2 O–Cu–SrTiO 3 three-phase interface in the hybrid is proved to play the key roles in the greatly enhanced electron transfer ability and the better catalytic activity. The present investigation indicates that the as-prepared samples may be effective and potential materials for the cleaner and sustained conversion of nitroarenes to aminoarenes on a lab level as well as a larger scale.
研究领域:
催化化学
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环境化学
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材料科学
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化学工程
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绿色化学
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Inorganic Chemistry Frontiers
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2022
·Vol. 10
·期 1
·240-249
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IF 7.779
Fangfang Chang,Yongpeng Liu,Juncai Wei,Lin Yang,Zhengyu Bai
Electrocatalytic CO2 reduction reactions (CO2RRs), an efficient method of converting carbon dioxide into valuable fuels and chemicals, are attractive as well as challenging. In this work, Cu2O nanostructures with active facets (face-raised cubic structures (F-Cu2O) with the (100) facet, octahedral structures (O-Cu2O) with the (111) facet and edge- and corner-truncated octahedral structures (T-Cu2O) with both the (100) and (111) facets) were synthesized by a wet chemical reduction method. The surface of Cu2O nanostructures was reconstructed in situ to form Cu2O/Cu with a highly active interface during the conversion of CO2 into C2H4, which is named F-Cu2O/Cu, O-Cu2O/Cu and T-Cu2O/Cu. The C2H4 selectivity on Cu2O/Cu catalysts follows the order of O-Cu2O/Cu < F-Cu2O/Cu < T-Cu2O/Cu, and the faradaic efficiencies of C2H4 are 11.2%, 24.9%, and 58.0% at −1.1 V versus the reversible hydrogen electrode, respectively. The experimental results combined with operando surface-enhanced Raman spectroscopy reveal that the Cu2O/Cu interface enhances *CO adsorption and decreases the activation energy of C–C coupling, which is also supported by density functional theory (DFT) calculations. This study will pave a feasible pathway for electrochemical energy storage and convention by crystal facet engineering and interface engineering.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Qiang Huang,Jiayu Yang,Fei Qi,Wenxia Zhang,Nan Zhang,Zhiyu Liang,Jiaxin Liu,Changqing Tian,Xiaosheng Tang,Daofu Wu,Benjun Huo
Photocatalytic conversion of CO 2 to value-added chemicals and fuels is a green and sustainable approach to solve the problems of CO 2 concentration increment and fossil fuels shortage. Employing photocatalysts with high catalytic activity and selectivity to realize CO 2 conversion has attracted extensive attention. However, the efficiency of photocatalysts is still unsatisfied and the selectivity of products is hard to be regulated, hindering their practical applications in large scale commercial purpose. In this work, for the first time, the Au and Pt was co-deposited on the heterostructure consisted of Cu 2 O quantum dots and ReS 2 nanosheets to achieve high efficiency and controllable selectivity during CO 2 photoreduction. The Au-Pt/Cu 2 O/ReS 2 photocatalysts show superior efficiency of CO 2 reduction than that of Au/Cu 2 O/ReS 2 , Pt/Cu 2 O/ReS 2 , Cu 2 O/ReS 2 , Cu 2 O. Such distinct improvement is attributed to the indirect Z-scheme mechanism and Schottky junction effect. Moreover, the synergetic effect of Au and Pt plays an important role of improving the photocatalytic activity, and the Au1-Pt5/Cu 2 O/ReS 2 exhibits the highest R electron of 516.86 μmol/g during one hour of visible light illumination, which is much larger than many recently reported photocatalysts under comparable condition. Meanwhile, the selectivity of CO and CH 4 is effortlessly tunable from 0 to 100% by modulating Au/Pt metal mass ratio due to the strong CO adsorption on Pt metals and the intensive interaction between Au and Pt atoms at the Au/Pt interface. This controllable selectivity provides admirable strategy to tune the component proportion of the gas products for the subsequent conversion into high value-added chemicals or liquid fuels. Our study proposes novel and deep insights into the design and fabrication of practical photocatalysts with high catalytic activity and controllable selectivity to perform efficient CO 2 photoconversion.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Xinxin Yuan,Jieyi Yang,Yiyang Yao,Hui Shen,Yue Meng,Bo Xie,Zheming Ni,Shengjie Xia
Single-phase photocatalysts exhibit low performance of photocatalytic degradation of pollutants, which is mainly due to the fact that most intrinsic photocatalysts can only produce one active species for degradation reactions. In order to solve this problem, the 0D/2D Cu 2 O/BiOCl S-scheme heterojunction was successfully constructed through a facile hydrothermal route. The obtained 0D/2D Cu 2 O/BiOCl displays high catalytic activity for tetracycline (TC) photodegradation, and 90.3% of TC was photodegraded within 80 min, which is much better than that by pure Cu 2 O and BiOCl. The excellent photocatalytic activity can be ascribed to the formation of S-scheme heterostructures, which enables the photocatalyst to generate superoxide radicals and hydroxyl radicals, and at the same time, makes the oxidation potential more positive and the reduction potential more negative. It is further proved by the results of experimental characterization and theoretical calculation show that the built-in electric field between Cu 2 O and BiOCl is a key factor in inducing the path of S-scheme electron transmission. In addition, the effects of various reaction conditions, including catalyst dosage, pH value and reaction temperature, on the photodegradation of tetracycline were discussed in detail. The intermediates and degradation path were also discussed in detail by liquid chromatography-mass spectrometry.
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ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Chaoyun Ma,Chulei Zhao,Chenglin Hong,Li Zhang,Siyu Chen,Yu Qi
The quantitative detection of carcinoembryonic antigen (CEA) indicators is a critical step in the early clinical diagnosis of cancer because CEA is closely related to the development of cancer. However, the most commonly used methods for CEA detection mainly involve comparing or measuring the color depth of colored substance solutions, which is not highly accurate, particularly when a second colored substance is present in the solution to be evaluated. Herein, we rationalized the design of a photothermal probe based on calcium carbonate (CaCO3) as a protective shell (Cu2O@CaCO3) for cuprous oxide (Cu2O) nanoparticles to prevent Cu2O oxidation and hyaluronic acid (HA) to confer material biocompatibility (Cu2O@CaCO3@HA). Cu2O can be specifically activated by hydrogen sulfide (H2S), transformed into Cu31S16 nanoparticles and display significant photothermal properties that can be visualized for bioanalysis by simply recording the temperature signal with a thermal imager. In addition, the presence of redox pairs can provide further electrochemically assisted validation of the temperature identification system. Given the portable, economical, and sensitive biosensing, we anticipate that future activatable nanoprobes may be used to assist in early cancer diagnosis and screening.
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ANALYTICA CHIMICA ACTA
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2021
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IF 6.558
Yang Zhao,Wei Zhao,Hong-Yuan Chen,Jing-Juan Xu
Nanoparticle plasmon scattering can provide real-time imaging information on the formation process of noble metal-based nanomaterials . Due to the synergistic effect of the interface between metal and oxide supporting pores, metal nanoparticles (NPs), especially Au NPs, generally exhibit higher catalytic activity on oxide carriers than single-component NPs. Here, we use the dark field scattering microscope to in situ monitor the growth of Au on Cu 2 O surface by oxidation-reduction reactions and the nanostructures could be precisely controlled via the scattering signal. The prepared Cu 2 O/Au nanocomposite has a higher electrocatalytic activity toward Glucose. When being used as a potential biosensor for nonenzyme glucose detection, excellent performance, such as high sensitivity with a detection limit of 4 μM, high selectivity and outstanding stability, was obtained. The scattering imaging strategy is a convenient and universal approach in controllable synthesis of plasmonic heterostructures, and leads to the improvement of electrocatalysts in biosensing.
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PubMed
高影响因子
APPLIED SURFACE SCIENCE
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2021
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IF 6.707
Xiaoxue Zhao,Linlin Sun,Xian Jin,Mengyang Xu,Shikang Yin,Jinze Li,Xin Li,Dong Shen,Yan Yan,Pengwei Huo
Z-scheme heterojunction can effectively separate photo-generated carriers and enhance photocatalytic activity of CO 2 reduction. In this work, we report indirect Z-scheme heterojunction of UiO-66-NH 2 /Cu 2 O/Cu, which achieves highly CO 2 photocatalytic conversion to CO. Among these, UiO-66-NH 2 /Cu 2 O/Cu-0.39 (U/C/Cu-0.39) displays the best activity with a CO yield of 4.54 μmol·g −1 ·h −1 , which is 37.8 times higher than that for UiO-66-NH 2 and 50.4 times higher than that for Cu 2 O. Cu not only acts as the electron conductor of the indirect Z-scheme heterojunction to promote the charge carrier transmission, but also acts as the active site of CO 2 reduction. The increase of active sites and the CO 2 adsorption capacity results in the superior photocatalytic performances.
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Journal of Materials Research and Technology-JMR&T
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2021
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IF 5.039
Chengli Yao,Xinna Gao,Xuan Liu,Yuhua Shen,Anjian Xie
It is a challenging and valuable work to synthesize surface enhanced Raman scattering (SERS) substrate with low cost and high performance by simple methods, and use it to detect pesticide residues in food. Here, Ferrero® chocolate-like Cu 2 O@Ag microspheres (FRC-Cu 2 O@Ag) were fabricated by a facile in-situ redox reaction. Cu 2 O directly acted as templates and reducing agents to induce the nucleation and growth of Ag nanoparticles on the microspheres surfaces. The prepared semiconductor-noble metal hybrids of Cu 2 O@Ag were utilized as SERS substrates to detect 4-mercaptobenzoic acid (4-MBA) and thiram molecules. The distinguished SERS effect was achieved when target molecules absorbed on the FRC-Cu 2 O@Ag composite. The substrate presented excellent sensitivity and reproducibility for the detection of 4-MBA and thiram with the limit of 10 −10 and 10 −9 M, respectively. Due to combining both advantages of electromagnetic enhancement of Ag metals and chemical enhancement of Cu 2 O semiconductors, the obtained FRC-Cu 2 O@Ag microspheres provided a SERS platform to conveniently detect molecules with thiol groups. When it was applied to detect thiram residues on apple peel and the detection limit was 1.2 × 10 −7 M, low than maximal residue limit (MRL) of 7 × 10 −6 M in fruit prescribed by the U.S. Environmental Protection Agency (EPA).
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Catalysts
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2020
·Vol. 10
·期 5
·539
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IF 3.52
Lan Luo,Tingting Zhang,Xin Zhang,Rongping Yun,Yanjun Lin,Bing Zhang,Xu Xiang
Hydrogen production by photoreforming of biomass-derived ethanol is a renewable way of obtaining clean fuel. We developed a site-specific deposition strategy to construct supported Au catalysts by rationally constructing Ti3+defects inTiO2nanorods and Cu2O-TiO2p-n junction across the interface of two components. The Au nanoparticles (~2.5 nm) were selectively anchored onto either TiO2nanorods (Au@TiO2/Cu2O) or Cu2O nanocubes (Au@Cu2O/TiO2) or both TiO2and Cu2O (Au@TiO2/Cu2O@Au) with the same Au loading. The electronic structure of supported Au species was changed by forming Au@TiO2interface due to the adjacent Ti3+defects and the associated oxygen vacancies while unchanged in Au@Cu2O/TiO2catalyst. The p-n junction of TiO2/Cu2O promoted charge separation and transfer across the junction. During ethanol photoreforming, Au@TiO2/Cu2O catalyst possessing both the Au@TiO2interface and the p-n junction showed the highest H2production rate of 8548 μmol gcat−1h−1under simulated solar light, apparently superior to both Au@TiO2and Au@Cu2O/TiO2catalyst. The acetaldehyde was produced in liquid phase at an almost stoichiometric rate, and C−C cleavage of ethanol molecules to form CH4or CO2was greatly inhibited. Extensive spectroscopic results support the claim that Au adjacent to surface Ti3+defects could be active sites for H2production and p-n junction of TiO2/Cu2O facilitates photo-generated charge transfer and further dehydrogenation of ethanol to acetaldehyde during the photoreforming.Keywords:ethanol reforming;hydrogen production;Au catalyst;Ti3+defect;site-specific deposition
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JOURNAL OF POWER SOURCES
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2020
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IF 8.247
Dongmei Zhuang,Xianli Huang,Zhihui Chen,Hao Gong,Lei Sheng,Li Song,Tao Wang,Jianping He
Lithium dendrite growth has long been regarded as the main obstacle for the practical usage of lithium metal battery . In this paper, we heat-treat the copper collector at a low temperature to prepare a Cu x O (x = 1–2)/Cu composite electrode. The samples heat-treated at 250 °C are mainly composed of Cu 2 O confirmed by X-ray photoelectron spectroscopy (XPS) analysis, which has the best wettability with propylene carbonate (PC)-based electrolyte. The as-prepared Li–Cu cell (composite electrode) can run more than 150 cycles. However, boric acid additive can prolong the cycle number of Li–Cu cell to more than 300 cycles at a current density of 0.5 mA cm −2 with a Coulombic efficiency larger than 85%. Scanning electron microscopy (SEM) image shows that the Cu 2 O/Cu composite electrode with boric acid additive in the electrolyte can inhibit the formation of lithium dendrite on the surface of the electrode, and a uniform and dense nano-columnar lithium layer can be obtained even at 5 mA cm −2 . The synergistic effect is attributed to the improved interfacial properties for Cu 2 O/Cu composite collectors when boric acid (BA) is used as additives.
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MICROCHIMICA ACTA
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2019
·Vol. 187
·期 1
·1-10
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IF 5.479
Li Yue,Wang Yan,Wang Mingchao,Zhang Jinyue,Wang Qingwei,Li Hongji
In a new method for the determination of trace levels of chlorophenols in river waters, detection via surface-enhanced Raman scattering (SERS) is combined with recognition by a molecularly imprinted polymer (MIP). Nanoparticles of type Cu 2 O@Ag were synthesized by attaching silver particles to the surface of Cu 2 O nanoparticles. The Cu 2 O@Ag were then coated with a layer of a MIP that was obtained by atom transfer radical polymerization using from methacrylic acid as monomers and 2,6-dichlorophenol as the template. The morphology of Cu 2 O is found to be flower-like. The Cu 2 O@Ag-MIPs displays a strong SERS effect. Following removal of the template by rinsing with the mixture solution of methanol/acetic acid (9/1, v /v), the material was used to selectively bind 2,6-dichlorophenol, 2,4-dichlorophenol and 2,4-dichlorophenol. The SERS peak intensity at 1580 cm −1 increases linearly with the concentration of the various chlorophenols in the range from 10 nM to 1 mM, and the detection limit is 5.8 nM. The imprinting factor is 4.62. The method was applied to the analysis of (spiked) river water, with recoveries ranging from 91.8 to 115.4% and relative standard deviations of <4.5%.
Graphical abstract
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PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 46
·18240-18250
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IF 3.069
Xiaoying Hu,Qi Zhang,Haoshan Nan,Ming Wang,Liang Qiao,Hongwei Tian
Compared to the traditional type II heterojunction photocatalyst (Cu2O/BiVO4), bulk BiVO4 was modified in this study by reduced graphene oxide (RGO) with a Schottky structure to optimize the coupling interface of BiVO4. Cu2O nanoparticles were then grown in situ on the RGO/BiVO4 surface to yield a heterojunction structure with an internal electric field, allowing movement of photogenerated electrons and holes in opposite directions to participate in redox reactions. The as-obtained optimized Cu2O/RGO/BiVO4 material exhibited excellent photocatalytic degradation performance towards organic pollutants. The reaction rate constant of rhodamine B (RhB) was estimated as 0.0324 min−1, which was almost 5.94, 5.15 and 1.94-fold higher than those of bare BiVO4, 4%RGO/BiVO4 and 5%Cu2O/BiVO4, respectively. Moreover, the optimized material displayed good activity in the degradation of the colorless organic contaminant tetracycline hydrochloride (TC). The reaction rate constant was estimated as 0.0219 min−1, which was almost 1.6-, 1.4- and 1.63-fold higher than those of bare BiVO4, 4%RGO/BiVO4 and 5%Cu2O/BiVO4, respectively. The hole and superoxide radical worked as active species for degradation of organic matter. Such a significant increase in degradation efficiencies was attributed not only to the formation of a heterojunction structure but also to rapid electron transfer between interfaces.
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