eScience
·
2023
·
IF 0
Mi Zhang,Meng Lu,Ming-Yi Yang,Jia-Peng Liao,Yu-Fei Liu,Hao-Jun Yan,Jia-Nan Chang,Tao-Yuan Yu,Shun-Li Li,Ya-Qian Lan
Electrocatalytic CO 2 reduction (ECR) to high value-added chemicals by using renewable electricity presents a promising strategy to realize “carbon neutrality”. However, the ECR system is still limited by its low current density and poor CO 2 utilization efficiency. Herein, by using the confinement effect of covalent organic frameworks (COFs) to confine the in-situ growth of metal nanoclusters (NCs), we develop a series of Cu NCs encapsulated on COF catalysts (Cu-NC@COF) for ECR. Among them, Cu-NC@CuPc-COF as a gas diffusion electrode (GDE) achieves a maximum CO 2 -to-CH 4 Faradaic efficiency of 74 ± 3% (at −1.0 V vs. Reversible Hydrogen Electrode (RHE)) with a current density of 538 ± 31 mA cm −2 (at −1.2 V vs. RHE) in a flow cell, making it one of the best among reported materials. More importantly, the current density is much higher than the relevant industrial current density (200 mA cm −2 ), indicating the potential for industrial application. This work opens up new possibilities for the design of ECR catalysts that utilize synergistic strategy.
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DOI
RSC Advances
·
2020
·Vol. 10
·期 47
·28059-28065
·
IF 3.119
Yunqi Fu,Mang Zheng,Qi Li,Liping Zhang,Shuai Wang,V. V. Kondratiev,Baojiang Jiang
Benzylamine coupling is a very important reaction for the synthesis of imine but still faces many challenges. Herein, we present a highly effective strategy towards the coupling reaction by using environmentally friendly catalysts. These catalysts are composed of Cu/Cu2O/Cu3N heterostructures supported by C3N4 tubes and the composites were synthesized by one-step hydrothermal treatment followed by calcination. Cu2O, Cu3N, and C3N4 all are responsive to visible light and the heterojunction formed can greatly enhance the charge separation. When used as photocatalysts for oxidative self-coupling of benzylamine at a low temperature of 323 K in air, Cu/Cu2O/Cu3N/C3N4 was able to give conversion and selectivity values of up to 99% and 98%, respectively. The high efficiency of the catalysts is attributable to their ability to generate large quantities of free radicals (such as ·OH and ·O2−) under visible-light irradiation.
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Yingying Yin,Lei Zhu,Tianchao Guo,Xurong Qiao,Shaopeng Gan,Xiao Chang,Xiaofang Li,Fujun Xia,Qingzhong Xue
The development of efficient oil/water separation membranes is highly significant for reducing severe environmental pollution nowadays. Constructing hierarchical structures with double-scale roughness and inverted trapezoidal geometry is an alternative rational design to fabricate low oil-adhesive membranes. Based on this design concept, a Cu mesh vertically wrapped with novel microphone-like Cu-CAT-1 hierarchical microstructures with double-scale roughness was tactfully prepared by a local concentration effect, which was referred to as CCMOF. The CCMOF possessed superior anti-oil-fouling performance and an outstanding water-absorbing capacity (180.3% larger than that of the pristine Cu mesh) due to its ingenious microphone-like structures and its high affinity for water. Therefore, it could separate various types of oil/water mixtures with a considerably high flux of over 25,000 L m −2 h −1 and an extremely low oil content in filtrate of below 10 ppm. The design concept of this work offered a simple idea to design low oil-adhesive membranes for efficient oil/water separation.
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DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Lu Long,Kaiji Xu,Kok Bing Tan,Dongren Cai,Yucheng Yang,Shu-Feng Zhou,Guowu Zhan
Catalytically agitating paddles are essential to perform liquid-solid heterogeneous catalytic reactions on an industrial scale due to the improved mass transfer and easy catalyst recovery. Herein, bimetallic oxides were formed after the calcination of nanomaterials derived from metal-organic frameworks (MOFs). Particularly, Mn(M)-BTC nanomaterials were synthesized by self-assembly of Mn 2+ ions (mixed with various dopants such as Cu 2+ , Ce 3+ , or Fe 2+ ) and H 3 BTC ligands in a mixed solvent of ethanol and water. It was found that in the powdery form, the Mn-Cu oxide derivate exhibited the highest degradation rate in the catalytic wet peroxide oxidation process (CWPO process), which was significantly higher than that of single metal oxide as well as Mn-Fe and Mn-Ce oxide derivates. The reason was caused by the synergistic effect between Mn-Cu promoted the formation of Mn 3+ and Cu + species to boost the CWPO reaction. Furthermore, the obtained Mn-Cu powdery catalysts were 3D-printed to obtain monolithic agitating paddles with different geometries, which were then mounted on a central shaft in the stirred reactor. An advanced oxidation process was used to investigate the effect of 3D patterns on the degradation efficiency of various organic dyes. It was discovered that the 3D-printed grid with higher cell density (484 cpsi) had better liquid mixing efficiency and thus better catalytic performance, which could be repeatedly used more than seven times. Additionally, the numerical simulation analysis (computational fluid dynamics) revealed a good mixing efficiency and improved mass transfer in the entire reactor equipped with the designed monolithic agitating impellers.
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DOI
高影响因子
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2021
·
IF 6.291
Xiaotian Zhou,Qilu Wang,Yuanming Guo,Xiumei Sun,Tiejun Li,Chenghu Yang
Dissolved organic matter (DOM) from macroalgae is regarded a crucial source of autochthonous DOM in coastal ocean. In the present study, the characteristics of DOM from the macroalgae Ulva pertusa decomposition ( U. pertusa -DOM) and its binding behaviors with Cu(II) using multiple spectroscopic techniques and chemometric analyses. The labile U. pertusa -DOM could be consumed and transformed by microorganisms. The absorption spectroscopic descriptors indicate that the hydrophobicity, aromaticity, and molecular weight of the U. pertusa -DOM increase during the 27-day incubation period. Fluorescence excitation–emission matrix spectroscopy combined with parallel factor analysis suggests that the relative abundance of the protein-like component (C1) (96.10–84.96%) sequentially decreases, whereas the humic-like components (C2) (2.16–9.73%) and (C3) (1.75–5.31%) in the U. pertusa -DOM increase with the U. pertusa decomposition. The Cu(II) binding properties of the U. pertusa -DOM are dependent on the decomposition time. The order of the conditional stability constant (log K M ) is C2 > C1 > C3. The complexation capacity ( f ) of C1 is higher than those of C2 and C3 at a specific time. Synchronous fluorescence spectroscopy coupled with two-dimensional correlation spectroscopy reveals that the microbial degradation could accelerate the Cu(II) binding to humic-like fractions in the U. pertusa -DOM. These findings will help us better understand the biogeochemical behaviors of macroalgal DOM and heavy metal in coastal ecosystems.
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DOI
高影响因子
Talanta Open
·
2022
·
IF 0
Jinping Yue,Qing Lv,Wan Wang,Qing Zhang
In this work, a new paper-based device (PAD) was developed for the colorimetric detection of multiple heavy metals. The sensing principle of this PAD is based on the analyte-regulated photocatalytic activity of quantum dots (QDs) to certain substrates. The PAD consisted of three filter paper layers, defining a sample area, three channels, and three testing areas. Three photocatalytic reactions between different QDs and their corresponding substrates could be performed in one device, achieving the simultaneous detection of Cu(II), Mn(II), and Hg(II). The detection limits are 7.3 nM for Cu(II), 5.4 nM for Mn(II), and 8.1 nM for Hg(II), respectively. This PAD was applied to analyze real samples and the results were consistent with those obtained by inductively coupled plasma-optical emission spectrometer. This approach may provide a promising colorimetric sensing platform for multi-target analysis.
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DOI
JOURNAL OF CATALYSIS
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2020
·
IF 7.888
Zhe Xu,Tiancheng Wu,Yu Cao,Congcong Chen,Xierong Zeng,Peng Lin,Wei-Wei Zhao
Production of multi-carbon (C 2+ ) products via electrochemical CO 2 reduction reaction (CO 2 RR) has aroused intensive interest in this decade. However, it is still a great challenge in large-scale synthesis of electrocatalysts for C 2+ compounds production with high selectivity and rate in neutral electrolyte. In this study, a robust and scalable aqueous synthesis method was proposed to prepare CuO nanosheets, which was directly used as CO 2 RR electrocatalyst. The catalyst underwent dynamic restructuring during the pre-reduction stage, which significantly changed the morphology, crystalline structure and electrochemical properties of the catalyst. As a result, the pristine CuO nanosheets gradually evolved to coral-like Cu nanoparticle ensembles (CL-Cu NEs). In 0.1 M KHCO 3 at −1.1 V vs. RHE, the CL-Cu NEs exhibited a faradaic efficiency and partial current density of C 2+ products of 72.1% and 25.2 mA cm −2 respectively and no degradation was observed in 15 h running. In contrast to many Cu-based catalysts showing considerable C 2+ products selectivity, the (sub)surface oxygen and Cu + species were unlikely to play a significant role in this study. The strong performance of CL-Cu NEs was ascribed to the synergism between the coral-like morphology and abundant Cu(1 0 0)/Cu(1 1 1) interfaces. This methodology may provide a cost-effective approach for large-scale preparation of CO 2 RR electrocatalysts with ideal nanostructure.
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DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2022
·
IF 10.319
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.
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DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2022
·
IF 3.656
Zhongjia Wu,Junlun Zhu,Wei Wen,Xiuhua Zhang,Shengfu Wang
4-Nitrophenol (4-NP) is water pollutant with good stability, high toxicity and difficult degradation, which will cause great harm to the environment. Thus, the development of high efficiency and rapid catalysts for the degradation of 4-NP will be an urgent problem to be solved. Herein, we synthesized covalent organic framework supporting Cu/Ag bimetallic nanoparticles (Cu/Ag–COF), which had better catalytic activity for the reduction of 4-NP. The porous COF possess large surface area of approximately 737.8 m 2 /g, so it can provide abundant sites for loading metal nanoparticles . At the same time, COF could also improve the stability and catalytic effect of nanocatalyst under flexible condition. The prepared Cu/Ag–COF exhibited the higher catalytic reduction of 4-NP into 4-aminophenol (4-AP) under the condition that the molar ratio of NaBH 4 to 4-NP was 147 and achieved an apparent rate constant of k Cu/Ag – COF = 0.0073 s −1 . The apparent rate constant of Cu/Ag–COF was higher than that of Ag–COF ( k Ag-COF = 0.0032 s −1 ) and Cu–COF ( k Cu-COF = 0.0047 s −1 ), indicating that this system had a synergistic catalytic effect to improve the catalytic activity of metal nanoparticles . Moreover, Cu/Ag–COF still had good catalytic effect after eight cycles, which indicated that it had good stability and reusability. This work provides a novel strategy to fabricate COF supported nanoparticles for outstanding performance in treating wastewater containing 4-NP.
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DOI
高影响因子
ChemCatChem
·
2020
·Vol. 12
·期 10
·2745-2751
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IF 4.853
Xinyang Guo,Fei Xue,Shikai Xu,Shaohua Shen,Hongwen Huang,Maochang Liu
Graphical How do you wave ? In this work, we realized the coupling of localized photothermal effect into a cocatalytic material by developing a unique core-shell Cu@Ni nanoplate cocatalyst for efficient photocatalytic H 2 production from water. Specifically, Cu nanoplate could induce localized hot spots on Ni nanoparticles via a visible-light-driven surface plasma resonance effect. As a result, photogenerated electrons transferred from g-C 3 N 4 to Ni, could be elevated to a more energetic state, leading to a substantially improved photocatalytic activity. The general moderate reaction condition in solar photocatalytic hydrogen production (i. e., near ambient pressure, room temperature) makes interfacial mass and energy transfer extremely slow, even by employing a cocatalytic material (usually in the form of noble metal nanoparticles or their counterparts). Herein, by fabricating well-defined Cu@Ni core-shell nanoplate cocatalyst and further incorporating it with a g-C 3 N 4 photocatalyst, we demonstrate that interfacial processes could be significantly improved by coupling localized photothermal effect into a cocatalyst. Specifically, Cu nanoplate can induce localized strong hot spots on Ni nanoparticles via a visible-light-driven surface plasma resonance effect. As a result, photogenerated electrons transferred from g-C 3 N 4 to Ni, could be elevated to a more energetic state, leading to a substantially improved photocatalytic activity toward H 2 evolution from water. The highest hydrogen generation rate reaches 55 μmol h −1 g −1 , 110 times of that pristine g-C 3 N 4 . This work indicates that photoelectric and photothermal effects can be effectively coupled by integrating metal hetero-nanoparticles.
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Ruyi Wang,Xianfeng Liu,Fu Yang,Shuying Gao,Shijian Zhou,Yan Kong
Herein, we report an efficient controlled approach to reach the synergetic neighboring dual-metal active sites in the confined mesopore of silica. In this approach, Mn-bearing mesoporous molecular sieve was designed in advance via a metal-assisted in-situ assembly route and further employed as a starting carrier to accommodate more extraneous Cu by impregnation. Controlling copper loading (Cu/Mn = 0.2, 0.4, and 0.6), comparative catalysts were attained and precisely characterized by key physicochemical methods. Impressively, in-situ formed highly-dispersed MnO x covered on the mesopore become the prerequisite for producing interplayed active species with neighboring dual Cu-Mn sites. Catalytic results concerning styrene epoxidation together with DRIFTS experiments and calculated bond energy variation in expected reaction intermediates demonstrated the existed synergy derived from formed neighboring Cu-Mn species via weakening and reinforcing appointed chemical bonds in intermediates. This study provides the foreseeable possibility for attaining universal synergetic catalysts in industrial heterogeneous catalysis.
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高影响因子
Energy Technology
·
2020
·Vol. 9
·期 1
·2000744
·
IF 3.404
Hai-Xu Zhao,Yi-Lin Liu,Gui-Gen Wang,Fei Li,Gui-Zhong Li,Hai-Ling Zhou,Hua-Yu Zhang,Jie-Cai Han
To meet the requirement of clean and efficient energy storage system for practical applications, supercapacitors (SCs), which are promising candidates for the next-generation energy storage devices, have received tremendous attention. Herein, a hybrid electrode consisting of copper nanowires (Cu NWs) and carbon nanotubes (CNTs) is prepared by simple vacuum-filtration method. Both Cu NWs and CNTs have excellent conductivities, high aspect ratios, and large surface areas, in which the two kinds of materials are evenly dispersed and are entangled with each other. The electrochemical performance characterization of the Cu@CuO NWs/CNTs hybrid electrode shows high specific capacitance of 1.7 F cm −2 and excellent cycling characteristics of 97.4% after 5000 cycles. The hybrid electrode of Cu@CuO NWs/CNTs with one-dimensional (1D) structure provides significant advantages in terms of electron/ion transport pathways. The SC devices with excellent electrochemical performance and stability clearly demonstrate their broad applications as low-cost, high-performance power supplies for electronic devices.
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DOI
高影响因子
危险品化学品经营许可证（带存储）