TOPICS IN CATALYSIS
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2023
·Vol. 66
·期 19
·1527-1538
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IF 3.6
Zhang Li,Men Yong,Wu Bin,Feng Yuanfen,Song Chao,Liu Shuang,Wang Jinguo,An Wei,Magkoev Tamerlan T.
Highly selective production of valuable ethylene from electrocatalytic CO 2 reduction reaction (ECO 2 RR) is particularly desirable yet challenging. Morphology engineering is an effective strategy for catalyst design, which can adjust the electronic structure of catalyst surface, change the adsorption behavior of critical reaction intermediates over catalyst surface, and thus regulate the activity of electrocatalytic CO 2 reduction reaction. In this work, we prepared copper phosphate catalysts with different morphologies and tested their catalytic activity for the ECO 2 RR in the flow cell. Compared with irregular flocculent aggregates, copper phosphate nanospheres exhibit a high and stable ethylene Faradaic efficiency of 47% with high current density of 350 mA·cm − 2 , which is higher than the 200 mA·cm − 2 required for industrial applications. The catalysts were extensively characterized by SEM, EDS, XRD, ICP-OES, XPS, BET and CO-TPD. Combining the characterization results and activity data, we found that the superior spherical morphology of copper phosphate can increase the electron density around Cu, stabilize the Cu + species on the surface through the electron transfer between P and Cu, and adjust the adsorption strength of CO intermediates (*CO) to enhance the productivity of C 2+ products. This work provides new insights into catalyst design for highly efficient C 2 H 4 production from the electrocatalytic CO 2 reduction reaction by tuning morphologies of Cu-based catalysts.
研究领域:
电化学
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材料科学
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催化
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Nano Research
·
2023
·
IF 9.9
Yang Limin,Qu Linjiao,Zhang Xiaolong,Li Mingming,Liu Zhen
Enzyme-inorganic hybrid nanoflowers (HNFs) have shown excellent sensing capabilities due to their large specific surface area as well as the simplicity and mildness of the preparation process. However, coupling HNFs to electrodes to fabricate a uniform and controllable enzymatic electrochemical sensing interface remains a challenge. Here, we proposed an aptamer-induced in-situ fabrication strategy for preparing an HNF-based electrochemical sensor with ideal performance. Central to this strategy is the introduction of acetylcholinesterase (AChE)-specific binding aptamer (Apt), which induces the in-situ growth of AChE-copper phosphate (Cu 3 (PO 4 ) 2 ) HNFs on the surface of carbon paper (CP). In addition, a dense gold nanoparticle (AuNP) layer was electrodeposited on the CP for anchoring Apt and further extending the electroactive surface area. The prepared AChE-Cu 3 (PO 4 ) 2 HNF/Apt/AuNP/CP biosensor exhibited a wide detection range from 1 to 10 7 pM for the four organophosphorus inhibitors, including isocarbophos, dichlorvos, methamidophos, and parathion, with detection limits down to 0.016, 0.028, 0.071, and 0.113 pM, respectively. With the reactivation of pralidoxime chloride, the electrode can still recover 98.1% of the response after five times of repeated use. In real sample detection, the biosensor achieved high recoveries from 96.45% to 100.13%. The detection target may be extendable to other AChE inhibitors (e.g., drugs for Alzheimer’s disease). This study demonstrates for the first time the feasibility of using aptamers as an inducer to fabricate an electrochemical enzyme sensing interface in-situ . This strategy can be used to fabricate other enzyme-based biosensors and therefore has broader applications.
研究领域:
分析化学
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生物传感器
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电化学
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纳米技术
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2019
·
IF 5.108
Linglu Gao,Qing He,Jinfeng Xing,Zhiqiang Ge
Doxorubicin (DOX) originated from users’ urine has been an emerging environmental pollutant due to its significant genotoxicity to mankind. Thus, urine source separation is a potential strategy to isolate DOX at a higher concentration and reduce the burden of downstream wastewater treatment . To develop highly efficient, easy separation and retrievable materials for individual patient to conveniently remove DOX from own urine, magnetic Cu 3 (PO 4 ) 2 nanoflowers were prepared through anchoring amino-functionalized magnetic nanoparticles on the Cu 3 (PO 4 ) 2 nanoflowers. Characterizations revealed the magnetic nanoflowers were spherical in shape with a mean size of 15 μm, and porous and hierarchical in structure. Magnetic nanoparticles located the surface of petals. Multibatch experiments were performed to assess the removal performance of DOX from aqueous solution. The magnetic nanoflowers exhibited excellent removal efficiency of DOX under weakly alkaline condition at ambient temperature. Linear and non-linear analyses were carried out to compare the best fitting kinetics and isotherms. Sorption kinetic data best fitted the pseudo-second order model. The Freundlich isotherm explained equilibrium sorption data with R 2 = 0.993 higher than that for the Langmuir isotherm. When the pH of synthetic urine was adjusted to weakly alkaline (pH 8.0–9.0), over 95% of DOX (20 mg L −1 ) was removed by a little of magnetic nanoflowers (50 mg L −1 ) within 5 min. Meanwhile, the magnetic nanoflowers could be easily separated and recovered from the synthetic urine by a magnet. So, for individual urine source separation strategy, the magnetic nanoflower seems to be an efficient, convenient and inexpensive approach to remove DOX from human urine.
研究领域:
环境科学
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纳米技术
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废水处理
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药物学
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材料科学
✓ 已验证
DOI
高影响因子
Analytical Methods
·
2022
·Vol. 14
·期 39
·3911-3920
·
IF 3.532
Limin Yang,Xiaolong Zhang,Mingming Li,Linjiao Qu,Zhen Liu
Immobilization of enzymes is one of the key steps in the development of high-performance enzymatic electrochemical biosensors, and various nanostructured materials have been designed and developed to achieve this goal. Herein, hybrid nanoflowers (HNFs) were synthesized using acetylcholinesterase (AChE) as an organic component and copper phosphate (Cu3(PO4)2) as an inorganic component. These AChE–Cu3(PO4)2 HNFs exhibit a three-dimensional hierarchical flower-like structure, which not only has a large specific surface area but also promotes the affinity between AChE and its substrate with better catalytic activity. Not only that, the surface modification of the glassy carbon electrode (GCE) by the joint use of gold nanoparticles (AuNPs) and graphene oxide (GO) extended the electroactive area. Using square-wave voltammetry (SWV), the as-prepared biosensor (i.e., AChE–Cu3(PO4)2 HNF/AuNP/GO/GCE) demonstrated superior sensing performance in the detection of dichlorvos. The detection limit is as low as 0.07 pM, and the linear detection range can range from 0.5 pM to 10 μM. In addition, the biosensor was feasible in real agricultural samples with satisfactory recoveries (98.65% to 103.43%). The reported biosensor provides an alternative tool for the direct measurements of AChE activity and its inhibition. Besides organophosphorus pesticides represented by dichlorvos, this biosensor has the potential to detect other AChE inhibitors, such as carbamate pesticides, drugs for Alzheimer's disease, etc., thus having broader applications in food safety and drug screening.
研究领域:
生物化学
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分析化学
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纳米技术
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROCHIMICA ACTA
·
2019
·Vol. 186
·期 7
·1-9
·
IF 5.479
Xu Lingling,Liu Zi,Lei Sheng,Huang Di,Zou Lina,Ye Baoxian
A sandwich-type electrochemical aptasensor is described for detecting the carcinoembryonic antigen (CEA) with high sensitivity and accuracy. Two kinds of nanomaterials are used. The first was obtained by modifying gold nanoparticles with reduced graphene oxide and hemin (Hemin-rGO-AuNPs). The second consists of horseradish peroxidase-modified organic-inorganic hybrid nanoflowers linked to gold nanoparticles to obtain an architecture of type HRP-Cu 3 (PO 4 ) 2 -HNF-AuNPs). These serve as carriers for two aptamers (apt1 and apt2) against CEA. Simultaneously, they were used to catalyze the precipitation reaction between 4-chloro-1-naphthol(4-CN) and H 2 O 2 . A sandwich-type assay linked to enzyme inhibition amplification was established for electrochemical determination of CEA. Under optimal experimental conditions and by using differential pulse voltammetry, the response peak currents (best measured at −0.34 V vs. Ag/AgCl) increases linearly with the logarithm of the CEA concentration in the range between 100 fg mL −1 and 100 ng mL −1 . The detection limit is as low as 29 fg mL −1 .
Schematic representation of the sandwich-type electrochemical aptasensor based on signal inhibition amplification from biocatalytic precipitation reaction. (HRP-Cu 3 (PO 4 ) 2 hybrid nanoflowers: Horseradish Peroxidase-Cu 3 (PO 4 ) 2 hybrid nanoflowers; AuNPs: Gold Nanoparticles; Hemin-rGO-AuNPs: Hemin-Reduced Graphene Oxide-Gold Nanoparticles; BSA: Bovine Serum Albumin; CEA: Carcinoembryonic Antigen; CEA apt1 : 5′-SH-(CH 2 ) 6 -ATA CCA GCT TAT TCA ATT-3′; CEA apt2 : 5′-NH 2 -(CH 2 ) 6 -AGG GGG TGA AGG GAT ACC C-3′; GCE: Glassy carbon electrode; 4-CN: 4-Chloro-1-naphthol; DPV: Differential pulse voltammetry).
研究领域:
生物化学
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分析化学
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纳米技术
·
癌症诊断
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）