Catalysts
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2021
·Vol. 11
·期 5
·535
·
IF 4.146
Shuaikang Zhu,Xiaona Ren,Xiaoxue Li,Xiaopo Niu,Miao Wang,Shuang Xu,Zheyuan Wang,Yunxi Han,Qingfa Wang
The copper-based catalyst is considered to be the only catalyst for electrochemical carbon dioxide reduction to produce a variety of hydrocarbons, but its low selectivity and low current density to C2products restrict its development. Herein, a core-shell xZnO@yCu2O catalysts for electrochemical CO2reduction was fabricated via a two-step route. The high selectivity of C2products of 49.8% on ZnO@4Cu2O (ethylene 33.5%, ethanol 16.3%) with an excellent total current density of 140.1 mA cm−2was achieved over this core-shell structure catalyst in a flow cell, in which the C2selectivity was twice that of Cu2O. The high electrochemical activity for ECR to C2products was attributed to the synergetic effects of the ZnO core and Cu2O shell, which not only enhanced the selectivity of the coordinating electron, improved the HER overpotential, and fastened the electron transfer, but also promoted the multielectron involved kinetics for ethylene and ethanol production. This work provides some new insights into the design of highly efficient Cu-based electrocatalysts for enhancing the selectivity of electrochemical CO2reduction to produce high-value C2products.Keywords:CO2electrochemical reduction;core-shell structure;ZnO@Cu2O;synergy effect;C2products selectivity
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ChemSusChem
·
2021
·Vol. 14
·期 15
·3190-3197
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IF 8.928
Wenwen Lin,Hao Chen,Zihao Li,Kotaro Sasaki,Siyu Yao,Zihao Zhang,Jing Li,Jie Fu
Graphical Yes, we CN : A simple and cost-effective method for the large-scale synthesis of Cu x O/CN catalysts is developed, involving high-temperature calcination with the aid of an N-rich component and anhydrous acetate. The CN film enriches the electron density at Cu x O metal active sites and Cu x O/CN shows a high C 2 H 4 faradaic efficiency of 42.2 %. The electroreduction of carbon dioxide to hydrocarbons has been proposed as a promising way to utilize CO 2 and maintain the ecosystem carbon balance. However, the selective reduction of CO 2 to C 2 hydrocarbons is still challenging. In this study, a highly efficient heterostructured catalyst has been developed, composed of a carbon nitride (CN)-encapsulated copper oxide hybrid (Cu x O/CN). The interaction between the metal and carbon nitride in the heterostructured catalysts improves the intrinsic electrical conductivity and the charge transfer processes at metal–support interfaces. A remarkable enhancement in the selectivity of hydrocarbons is achieved with these modified Cu-based electrocatalysts, with an onset potential of −0.4 V and high C 2 H 4 faradaic efficiency of 42.2 %, and these catalysts can also effectively suppress H 2 evolution during the CO 2 reduction reaction. This work provides a simple and cost-effective method for synthesizing CN-encapsulated catalysts that provides the possibility of efficiently converting CO 2 into C 2 hydrocarbons.
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ACS Applied Nano Materials
·
2021
·
IF 5.097
Lin Guo,Zhu Mao,Chao Ma,Jiawei Wu,Lin Zhu,Bing Zhao,Young Mee Jung
Nanoscale materials have an irreplaceable advantage in solar energy utilization because of their perfect match with visible light wavelength on the length scale. Charge transfer (CT) between a metal nanoparticle and contacted nanoscale semiconductor plays a significant role in photoinduced energy transfer. Here, we fabricated a new complex, a gold nanorod-4-mercaptobenzoic acid@Cu2O (Au NR-MBA@Cu2O) core–shell nanostructure, and used surface-enhanced Raman scattering (SERS) spectroscopy of the interlayer MBA molecules to investigate the CT process occurring between the Au NRs and Cu2O. In our system, different surface plasmon absorption bands were adjusted by tuning the thicknesses of the Cu2O shells on the Au NR core to explore the influence of plasmon absorption at different incident Raman laser lines. By analyzing the SERS spectra, the degree of CT was calculated, and the consequences can be fully explained by photoexcitation across interface electron transfer and plasmon-induced interfacial charge transfer transition at laser excitation wavelengths of 633 and 785 nm. This experiment introduced a simple, effective, and intuitive approach to observe the CT process in metal semiconductors by SERS. The results of our study will improve in photocatalytic efficiency and photoelectric devices.
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CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Bo Ma,Jinglei Bi,Jian Lv,Chuncai Kong,Pengxu Yan,Xintian Zhao,Xiaojing Zhang,Tao Yang,Zhimao Yang
Constructing the heterostructure with noble metals on semiconductors is recognized as a prospective approach to enhance hydrogen generation. In this study, Au-Cu 2 O heterostructure particles (HPs) with unique inter-embedded heterostructures were controllably fabricated by a universal reaction between Cu particles and HAuCl 4 solution. Besides, the boosted catalytic performance from the plasmon effects, Au-Cu 2 O inter-embedded heterostructure exhibits additional structural advantages to promote the photocatalytic property of hydrogen generation overall water splitting. Under the visible light, the H 2 evolution rate of the Au-Cu 2 O HPs is 152 and 22 times higher than that of pure Cu 2 O and traditional Cu 2 O@Au HPs with Au anchored on the surface of Cu 2 O, respectively. On one hand, inter-embedded heterostructure brings more contact areas as the active sites to carry out the direct electron transfer and electromagnetic transfer for the reduction. On the other hand, the finite difference time domain (FDTD) simulations indicate that enhanced electromagnetic fields of Au-Cu 2 O HPs form a netlike structure to maximumly accelerate the transfer of hot electrons and separate the electron–hole pairs. Under the joint action of the two, the inter-embed heterostructure exhibits superior photocatalytic property, demonstrating that this study could instruct the design of other metal–semiconductor photocatalysts.
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APPLIED SURFACE SCIENCE
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2020
·
IF 6.182
Yi Zhang,Qi Wang,Dongming Liu,Qian Wang,Tong Li,Zhou Wang
A novel isotype (p-p) heterojunction, on the basis of Cu 2 O coupled with BiOI, has been designed and synthesized via a facile two-step electro-deposition approach at room temperature. The morphology, phase compositions and chemical bonding state were verified by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction measurements (XRD) and X-ray photoelectron spectra (XPS). The optimized Cu 2 O/BiOI hybrid electrode exhibited boosted photoelectrochemical (PEC) H 2 O 2 non-enzymatic sensing performance under visible light illumination, with a phenomenally broad linear range (1.99 µM ~ 17.54 mM), a high sensitivity of 213.87 µA mM −1 cm −2 , as well as a low detection limit of 0.44 µM (S/N = 3). Additionally, the sensor presented satisfying selectivity, repeatability, stability and its feasibility in real samples was corroborated. The photoelectrochemical sensing mechanism was clarified in the view of band structure and p-p heterojunction. Our work would enlighten the perspective research on the application of isotype heterojunction in PEC bio-sensing and provide a promising non-enzymatic biosensor platform for effective detection of H 2 O 2 in food, biomedical and environment analysis.
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RSC Advances
·
2019
·Vol. 9
·期 63
·36831-36837
·
IF 3.049
Xiaodong Yang,Shupeng Zhang,Lei Zhang,Bo Zhang,Tianrui Ren
Compared with low-index {100} or {111} planes of Cu2O crystals, rhombic dodecahedra (RD) Cu2O crystals exposing 12 {110} facets exhibit the most superior photodegradation of organic pollutants. Herein, a series of RD Cu2O crystals with different sizes were successfully synthesized by precisely adjusting the reaction temperature ranging from 40 °C to 100 °C. The results revealed that truncated rhombic dodecahedra (TRD) Cu2O crystals were fabricated when the temperatures was 40 °C. More importantly, on raising the temperature to above 40 °C, Cu2O architectures dynamically evolved from TRD to RD. Meanwhile, the sizes gradually decreased with elevation of the temperature, while the RD morphology of Cu2O crystals remained, demonstrating the importance of temperature for determining the morphology and size of Cu2O crystals. In addition, we also carefully investigated the visible-light photodegradation performance of Cu2O crystals for methyl orange (MO). RD Cu2O crystals exhibited superior photocatalytic activity compared with TRD, and showed size-dependent photocatalytic activity for MO. The photocatalytic activity of RD Cu2O crystals can be greatly improved by decreasing the size. In particular, RD-60 with the minimum size achieved the best photocatalytic properties compared to the other RD and TRD Cu2O crystals, and still displayed high photocatalytic efficiency even after three cycles. Such results advance the understanding that temperature modulation serves as an effective means to fabricate RD Cu2O crystals.
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Journal of CO2 Utilization
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2019
·
IF 5.189
Miao Wang,Xiaona Ren,Gang Yuan,Xiaopo Niu,Qingli Xu,Wenluan Gao,Shuaikang Zhu,Qingfa Wang
Element doping is an effective strategy to enhance the selectivity of electrochemical carbon dioxide reduction. In this work, a dendritic core-shell In-doped Cu@Cu 2 O catalyst is prepared by co-electrodeposition method on carbon fiber paper for selective electroreduction of CO 2 to CO. Faradaic efficiency of producing CO over this dendritic In-doped Cu@Cu 2 O reaches 87.6 ± 2.2% with total current density of 11.1 ± 0.85 mA cm −2 at −0.8 V vs RHE, which outperforms most of the reported Cu-based electrocatalysts. The excellent performance is mainly derived from charge re-distribution and the enhanced intrinsic activity due to the formation of In-doped Cu 2 O layer. Meanwhile, the Cu + /Cu 0 can be adjusted by tailoring the doped-In content. The relatively high ECSA and small charge transfer resistance are also conducive to improve the selectivity and activity. The oxyphilic In metal incorporated into the copper lattice can well stabilize the intermediate *COOH through enhancing interaction with O-ends of *COOH. This work provides a facile approach and a deep insight on design and synthesis of high efficiency hybrid electrocatalysts.
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Photonics and Nanostructures-Fundamentals and Applications
·
2018
·
IF 1.575
Xiaofeng Wei,Jiaqi Pan,Jie Mei,Yingying Zheng,Can Cui,Chaorong Li
The orderly nano array is able to improve the light utilization efficiency and has been thought to be a promising way for advancing photocatalysis. The orderly nano array of truncated octahedra Cu 2 O nanocrystals have been successfully fabricated by the facile solution-based one-step reduction and self-assembly method. The results of XRD, SEM and TEM indicate that the Cu 2 O nano array is successfully assembled on the Si substrate. The photocatalytic activity of the Cu 2 O orderly nano array is investigated under visible light irradiation, and it is demonstrated to be significantly enhanced after the Cu 2 O is self-assembled orderly. Furthermore, the surface orderly structure of the nano array is considered as the main reason for the enhancement.
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CRYSTENGCOMM
·
2018
·Vol. 20
·期 41
·6580-6588
·
IF 3.304
Pengwei Li,Dingding Li,Lina Liu,Anli Li,Cuixian Luo,Yue Xiao,Jie Hu,Huabei Jiang,Wendong Zhang
In this work, a concave structure of Cu2O truncated microcubes with {100} facet erosion has been successfully synthesized by a facile top-down etching method. Air and PVP were employed as an etchant and a shape controller agent, respectively. For the facet-selective capping of PVP on Cu2O {111} planes, the traditional relatively low energy {100} facets of Cu2O truncated microcubes would be selectively etched along their [100] zone axis in a top-down manner. The {100} facet etched Cu2O concave truncated microcubes exhibited highly improved photocatalytic activities (2.15 and 1.21 times, respectively) compared to that of the basic structure and the {111} facet etched samples on the degradation of Congo red (CR), displaying distinct facet-dependent photocatalytic characteristics, excellent stability and reusability. This work not only builds an efficient photocatalyst, but also provides a novel method to fabricate a variety of architectures with low energy facets etched and highly active crystal planes exposed, which is extremely important for the improvement of catalytic activities.
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BIOSENSORS & BIOELECTRONICS
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2015
·
IF 6.409
Hongmin Ma,Yan Li,Yulan Wang,Lihua Hu,Yong Zhang,Dawei Fan,Tao Yan,Qin Wei
In this work, an ultrasensitive sandwich-type electrochemical immunosensor was developed for the quantitative detection of prostate specific antigen (PSA). Gold nanoparticles decorated 3-aminopropyltriethoxysilane functionalized graphene sheets (Au@APTES-GS) with a large specific surface area, good biocompatibility and superior electron transfer ability were employed as the matrix. In addition, cubic Cu 2 O nanoframes with hollow edges were employed as the label for the first time. Scanning electron microscope (SEM) images were used to confirm the nanostructure of Au@APTES-GS and Cu 2 O. Using square wave voltammetry (SWV) to monitor the electrocatalytic process, the signal amplification mechanism of the matrix and the label were explored successfully. Here we find that the unique edge-truncated structure of Cu 2 O nanoframes can load with a larger amount of redox mediators , ferrocenecarboxylic acid (Fc-COOH), offering a higher electrochemical signal response. Apart from that, Cu 2 O nanoframes have a good electrocatalytic activity towards the Fc-COOH and hydrogen peroxide (H 2 O 2 ), making a contribution to further enhance the sensitivity of the fabricated immunosensor. Under optimal conditions, the proposed immunosensor achieved an ultrasensitive and specific detection of PSA, and displayed acceptable reproducibility, selectivity and stability. This work may provide an effective method for the clinical monitoring of tumor markers and demonstrate the potential application promising of nanoframes in the fabrication of immunosensors.
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ELECTROCHIMICA ACTA
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2013
·
IF 3.777
Dan-Ling Zhou,Jiu-Ju Feng,Lin-Yi Cai,Qin-Xue Fang,Jian-Rong Chen,Ai-Jun Wang
In this work, well-defined monodisperse porous Cu 2 O nanospheres were facilely synthesized, using ionic liquid crystal 1-hexadecyl-2,3-dimethylimidazolium bromide ([C 16 MMIm]Br) as a soft template. The as-prepared Cu 2 O nanospheres were successfully anchored on the reduced graphene oxide nanosheets (RGOs) by simple ultrasonication. The RGOs-Cu 2 O nanocomposites showed high electrocatalytic activity toward glucose oxidation. Thus, a non-enzymatic amperometric glucose sensor was constructed with a wide linear range from 0.01 to 6 mM, low detection limit of 0.05 μM ( S/N = 3), high selectivity (185 μA mM −1 ), and fast response (within 3 s). This strategy opens a new facile and simple chemical route to prepare porous metal oxides supported on RGOs with novel properties.
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RSC Advances
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2015
·Vol. 5
·期 43
·33938-33945
·
IF 3.84
Chunbo Liu,Ping Li,Guoling Wu,Bifu Luo,Shuang Lin,Ao Ren,Weidong Shi
In our study, a new visible-light-driven photocatalyst Cu2O/SrTiO3 (C/S) heterojunction was firstly prepared by a simple, facile and effective deposition–precipitation technique. The particle size of the Cu2O nanoparticle is only about 5 nm and the SrTiO3 (STO) nanocube is about 50 nm when modified by Cu2O nanoparticles. The samples are used as photocatalysts for photodegrading tetracycline (TC) under visible light irradiation. The 9-Cu2O/SrTiO3 (9-C/S) sample heterojunction shows the highest TC degradation ratio (77.65%), which is caused by the photogenerated electrons of the Cu2O nanoparticles moving from the conduction band of Cu2O to that of SrTiO3, resulting in the separation of electrons and holes. This study not only shows a possibility for substituting noble metals with low-cost Cu2O nanoparticles in photocatalytic degradation but also exhibits a facile deposition–precipitation technique for synthesizing narrow/wide band gap photocatalysts.
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