Journal of Materials Chemistry B
·
2020
·Vol. 8
·期 37
·8599-8606
·
IF 5.344
Zhen Lin,Linlin Zheng,Wensong Yao,Shijun Liu,Yemei Bu,Qi Zeng,Xiaomin Zhang,Haohua Deng,Xinhua Lin,Wei Chen
Nanozymes have emerged as enzyme-mimicking nanomaterials to overcome the low stability and high cost of some natural enzymes. The design and fabrication of nanozymes with superior performance to natural enzymes are in urgent demand. Single-atom catalysts offer the unique characteristics of maximum atomic utilization, and are an excellent candidate for nanozymes. However, most of the reported synthesis methods for single-atom catalysts require the preparation of supports for single-atom catalysts in advance, which requires multiple steps and calcination in a high temperature atmosphere. Herein, Cu–N–C single-atom nanozymes (Cu–N–C SAzymes) were successfully designed via a one-pot solvothermal method. Cu–N–C SAzymes exhibited excellent peroxidase-mimicking activity that is superior to some other related nanoparticles. The mechanism study revealed that H2O2 was catalyzed by Cu–N–C SAzymes to generate reactive oxygen species. Furthermore, based on the excellent peroxidase-mimicking activity of the Cu–N–C SAzymes, a simple and sensitive detection method for H2O2 and glucose has been developed.
研究领域:
纳米技术
·
催化
·
生物化学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Materials Today Chemistry
·
2024
·
IF 6.7
Yiting Jiang,Zhejie Chen,Yating Yuan,Linxin Tian,Chuhuang Dong,Wencheng Shen,Jinchao Wei,Shengpeng Wang,Yu Yang,Jia Ge
Alpha-glucosidase (α-Glu) is a hydrolase that promotes the rise of glucose in the blood during the digestion process, and it plays a crucial role in regulating glucose levels within a normal range. Herein, we developed an ultrasensitive colorimetric platform by preparing a Cu–N–C single-atom nanozyme (Cu–N–C SAzyme) with a potent oxidase-like effect on accurately detection of α-Glu and efficient screening of its potential inhibitors. This artificial nanoenzyme was able to catalyze the oxidation of colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to blue oxide (oxTMB) without the assistance of H 2 O 2 . In addition, with the participation of α-Glu, l -ascorbic acid-2- O -α- d -glucopyranose (AAG) can be catalyzed to produce ascorbic acid (AA), which significantly reduces the oxidation, resulting in a noticeable fading of the blue color. Therefore, we designed a straightforward colorimetric test for α-Glu activity, achieving detection limits as low as 0.09 U/L and a linear response from 0.25 to 8 U/L. Most importantly, this platform has been effectively applied to measure α-Glu in real samples.
研究领域:
生物化学
·
医学诊断
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2023
·Vol. 170
·期 7
·077509
·
IF 3.9
Qi Wang,Wenjing Liu,Jinjin Zhang,Jianying Qu
In this work, Cu/N-C derived from MOF composites were synthesized and characterized by SEM, XRD, FTIR, XPS and EIS, which was modified on the glassy carbon electrode (GCE) to construct a novel electrochemical sensor (Cu/N-C/GCE). Due to the good electrical conductivity and abundant catalytic active sites of Cu/N-C, Cu/N-C/GCE exhibited excellent electrocatalytic performance for catechol (CC) and hydroquinone (HQ) with the oxidation peak potential difference of 112 mV. The proposed sensor could realize the simultaneous detection of CC and HQ successfully. Under optimal conditions, the redox peak currents of both CC and HQ have good linear relationship with their concentrations in the ranges of 0.50–100.00 μM and 0.50–150.00 μM with the detection limits for CC and HQ of 0.12 μM and 0.09 μM, respectively. At the same time, the sensor exhibits good stability, reproducibility and selectivity in the analysis of practical samples.
研究领域:
分析化学
·
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Linzhi Shen,Ziwen Xiong,Zhaohui Du,Hao Wang,Wenrui Li,Zhen Zhang,Hao Wu,Changsong Zhou,Yaming Zhou,Guanghua Tang,Jing Liu,Hongmin Yang
M-N-C catalysts have considerable potential in the fields of catalysis, such as highly polluting gaseous elemental mercury (Hg 0 ) oxidation. However, the direct application of these kinds of catalysts for mercury removal is stymied by their low catalytic efficiency. Heteroatom-doping in M-N-C catalysts has been proposed as a powerful strategy to the promote catalytic of Hg 0 , but the origin of boosting catalytic activity is still elusive. Herein, it is disclosed that selenium doping induces an obvious electron-acceptor effect for accelerating the Hg 0 catalytic oxidation. The model selenium-doped Cu-N-C catalyst with atomically dispersed active sites was verified by various characterization methods, such as SEM-EDS and scanning transmission electron microscopy. The optimal Cu-NC-Se with Cu/Se ratio of 1:1 exhibited the best Hg 0 removal performance, over 8-fold enhancement in their Hg 0 oxidation capacities than raw selenium-free Cu-NC. At the optimal reaction temperature of 90 °C, Cu-NC-Se achieved an average Hg 0 removal rate of 92.44% within 60 min under single pure N 2 atmosphere. As for the influence of flue gas components, the presence of O 2 promoted the removal of mercury in Cu-NC-Se, whereas CO 2 , NO and SO 2 served as slight inhibitors. Even after five cycles of the experiment, the average mercury oxidization efficiency was still remained at 88.5%, showing that Cu-NC-Se can be reused with good maintenance of the catalytic activity and atomic dispersion of Cu and Se in the structure. The unsaturated Cu sites connected with pyridinic N on the carbon matrix can serve preferential adsorption to Hg 0 and doped selenium. Meanwhile, the selenium doping accelerated Hg 0 adsorption and accept sufficient electrons for promoting Hg 0 oxidation to forming stable HgSe, which is also corroborated by the theoretical analysis results based on density functional theory. This work not only provides an alternative facile synthetic strategy for developing heteroatom-doping atomically dispersed M-N-C catalysts, but also represents a significant advance for deepening the understanding of the Hg 0 catalytic oxidation mechanism on M-N-C catalyst.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Surfaces and Interfaces
·
2025
·
IF 6.3
Xiaoyang Fan,Pengfei Wu,Chao Qu,Ziqian Shi,Ruidong Wang,Yansheng Sun,Tingting You,Yukun Gao,Penggang Yin
Photo-induced Metal-Catalyzed Radical Polymerization (PMCR) of nitroaromatic compounds represents a highly effective strategy for synthesizing aromatic azo compounds, with broad applications across materials science, medicine, and agricultural chemistry. Cu/N/C nanosheets (NSs) substrates were prepared through thermal decomposition from Cu-based Metal-Organic Frameworks (MOFs). PMCR of 4-Aminothiophenol (PATP) to 4,4′-Dithiodianiline (DMAB) was in situ monitored on the prepared substrates by Raman spectroscopy technique. It exhibit efficient localized surface plasmon resonance effects with over 10 5 Raman enhancement factor, significantly promoting the conversion of PATP to DMAB under an applied electric field. It is attributed to the adjustment of the energy band structure of the material through N-doping and the precise control over the valence state of Cu elements within the material. This research presents a highly simple, efficient, and cost-effective strategy for accelerating the coupling reaction of nitroaromatic compounds, while also proposing a novel approach for monitoring plasma-interface reactions.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-13
·
IF 14.7
Li Yifan,Huang Aijian,Zhou Lingxi,Li Bohan,Zheng Muyun,Zhuang Zewen,Chen Chang,Chen Chen,Kang Feiyu,Lv Ruitao
Developing highly active and durable air cathode catalysts is crucial yet challenging for rechargeable zinc-air batteries. Herein, a size-adjustable, flexible, and self-standing carbon membrane catalyst encapsulating adjacent Cu/Na dual-atom sites is prepared using a solution blow spinning technique combined with a pyrolysis strategy. The intrinsic activity of the Cu-N 4 site is boosted by the neighboring Na-containing functional group, which enhances O 2 adsorption and optimizes the rate-determining step of O 2 activation (*O 2 → *OOH) during the oxygen reduction reaction process. Meanwhile, the Cu-N 4 sites are encapsulated within carbon nanofibers and anchored by the carbon matrix to form a C 2 -Cu-N 4 configuration, thereby reinforcing the stability of the Cu centers. Moreover, the introduction of Na-containing functional groups on the carbon atoms significantly reduces the positive charge on their outer shell C atoms, rendering the carbon skeletons less susceptible to corrosion by oxygen species and further preventing the dissolution of Cu centers. Under these multi-type regulations, the zinc-air battery with Cu/Na-carbon membrane catalyst as the air cathode demonstrates long-term discharge/charge cycle stability of over 5000 h. This considerable stability improvement represents a critical step towards developing Cu-N 4 active sites modified with the neighboring main-group metal-containing functional groups to overcome the durability barriers of zinc-air batteries for future practical applications.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nano Energy
·
2017
·
IF 12.343
Wenjun Fan,Zelong Li,Chenghang You,Xu Zong,Xinlong Tian,Shu Miao,Ting Shu,Can Li,Shijun Liao
In this work, CuCl 2 as a promoter was added into the mixture of polythiophene (PTh), FeCl 3 , and melamine for preparing Fe-Cu-N/C catalyst. The catalyst features one-dimensional bamboo-like carbon nanotubes with few metal oxide nanoparticles encapsulated into tubes. The catalyst exhibits excellent activity toward the oxygen reduction reaction (ORR) with half-wave potential 50 mV more positive than the commercial Pt/C in 0.1 M KOH. It also shows comparable ORR activity in 0.1 M HClO 4 solution. Moreover, it exhibits superior long-term stability and excellent methanol tolerance in both alkaline and acidic solutions. The outstanding catalytic performance of Fe-Cu-N/C catalyst can be ascribed to the doping of Cu in the Fe-N-C architecture, which promotes the formation of bamboo-like nanotube structure and the generation of interaction among Cu and Fe-N-C. This synthetic strategy may open new avenues for constructing highly efficient electrocatalysts that adding of an inactive metal can obviously promote the catalytic performance of catalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Hanjun Zhang,Jing Chen,Yuxin Shi,Yaoyue Yang,Xiaole Jiang
Regulating the local microenvironment of metal centers represents an effective yet challenging approach to enhance the catalytic performance of atomically dispersed transition metal-nitrogen-carbon (M–N–C) catalysts towards the oxygen reduction reaction (ORR). Herein, atomically dispersed Cu–N–C catalysts featuring with adjustable carbon vacancies/defects concentrations (Cu–N–C V –X) are fabricated using a simple molten-salt-assisted pyrolysis strategy. The optimized catalyst (Cu–N–C V -1000) exhibits superior ORR catalytic performance with a half-wave potential ( E 1/2 ) of 0.89 V versus the reversible hydrogen electrode (RHE) and a turnover frequency ( TOF ) of 5.01 e site -1 s −1 at 0.85 V, surpassing Pt/C and most recently reported single-atom catalysts. Theoretical calculations confirm that defects adjacent to Cu–N 3 site downshift the d-band center of active sites, facilitating the desorption of *OH intermediate and thereby significantly enhancing the ORR kinetics. Consequently, the Cu–N–C V -1000-based zinc-air battery (ZAB) delivers a peak power density of 175.0 mW cm −2 along with a high discharge specific capacity of 819.4 mA g -1 Zn . This work confirms that the deliberate creation of suitable defects is an effective approach to optimize the intrinsic ORR activity of atomic M–N x sites, providing new insights into the rational design of high-performance catalysts for practical metal-air batteries.
研究领域:
材料科学
·
电催化
·
能量存储与转换
·
纳米技术
·
理论化学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2021
·Vol. 14
·期 5
·1796-1806
·
IF 7.79
Wenyan Yin,Milin Zhang,Jingyuan Liu,Khaled Tawfik Alali,Jing Yu,Jiahui Zhu,Peili Liu,Rumin Li,Jun Wang
Electrochemical sensors using ionic liquids as electrolytes for oxygen detection are now getting more and more attention. Recently, an ionic liquid combined with an electrochemically active catalyst system has become popular for boosting the sensing performance of oxygen sensors. In this work, the imidazolyl-based ionic liquid 1-butyl-2,3-dimethylimidazole bis((trifluoromethyl)sulfonyl)imide [Bmmim][TFSI] is first prepared by a facile two-step method. Subsequently, a transition metal and N-codoped porous carbon oxygen reduction electrochemical catalyst Cu–N/C is synthesized by calcining the Cu-doped ZIF-8 precursor and then blending it in different ratios with the ionic liquid [Bmmim][TFSI] as composite electrolytes for oxygen detection. The composite electrolyte Cu–N/C/[Bmmim][TFSI] exhibits increased responses in cyclic voltammetry (CV) and chronoamperometry (CA) relative to that of the pure ionic liquid. Furthermore, the CV and CA data show that 6% Cu–N/C/[Bmmim][TFSI] has the optimum oxygen sensing response with an enhanced reduction peak current, a sensitivity of 0.1678 μA/[% O2] and a good linear fitting coefficient of 0.9991. In conclusion, the results confirm the success of using Cu–N/C as an electrochemical catalyst composed of the Cu–N/C/[Bmmim][TFSI] electrolyte for improving the responsivity, stability and sensitivity towards a wide range of oxygen concentrations.
研究领域:
材料科学
·
电化学
·
环境监测
✓ 已验证
产品关联
DOI
PubMed
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Huiqian Yang,Min Wang,Tingting Yang,Chunxia Li,Aifeng Li,Jinsheng Zhao
This paper mainly uses the molecular recognition principle and synergistic effect to synthesize the functional supramolecular 2,7-bis(4-([2,2':6',2''-terpyridin]-4'-yl)phenyl)-9-(heptadecan-9-yl)-9 H -carbazole. The nitrogen active sites at both ends of terpyridine are coordinated with metal copper ions to form a metal supramolecular catalyst that contains both the metal and nitrogen active sites. The surface physical structure and elemental analysis of the synthesized complexes were analyzed using SEM and XPS. The redox properties of the catalysts were characterized using chemical characterization methods, such as cyclic voltammetry (CV), linear sweep voltammetry (LSV), and a rotating ring disk electrode (RRDE). The physical and chemical analysis showed that the catalyst was successfully synthesized and that it was subjected to a redox reaction via a four-electron process. Therefore, the prepared metal supramolecular catalyst has good catalytic performance.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2024
·
IF 5.7
Mengqiong Zhang,Guowen Wang,Jiping Chen,Xianbo Lu
Bisphenol compounds (BPA, BPS, BPAF, etc.) are one class of the most important and widespread pollutants that poses severe threat to human health and the ecological environment. Because of the presence of multiple bisphenols in environmental and food samples, it is urgent and challenging to develop a rapid and cheap technique for simultaneously detecting BPA and its analogues. In this study, a series of M - N -C (M = Cu, Mg, Ni, Co, Fe, K) single-atom nanozymes (SAzymes) were created by simulating the structure of natural enzyme molecules, which were used as novel sensing platform for the fabrication of electrochemical sensors. Through systematic screening and characterization, it was interestingly discovered that the electrochemical sensor based on Cu- N -C SAzymes exhibited the best sensing performance for bisphenols among all SAzymes, which catalyzed not only BPA like tyrosinase, but also showed excellent catalytic capacity beyond tyrosinase (tyrosinase has no catalytic activity for BPS, BPAF, etc.), and achieved potential-resolved simultaneous rapid detection of BPA, BPS and BPAF. Further structure-activity relationship and catalytic mechanism characterizations of Cu- N -C SAzymes revealed that the presence of single atom Cu was predominantly in the form of Cu + and Cu 2+ , which were anchored onto graphene nanosheet support through four coordination bonds with pyridinic N and pyrrolic N and acted as highly efficient active centers for electrocatalytic oxidation of bisphenols. The developed electrochemical sensing method exhibited excellent selectivity, sensitivity, and reliability for the rapid detection of multiple bisphenols in actual samples.
研究领域:
分析化学
·
环境科学
·
材料科学
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2020
·
IF 4.473
Liting Cui,Zhengjian Li,Haining Wang,Lirui Cui,Jin Zhang,Shanfu Lu,Yan Xiang
It is of great significance to reduce the amount of platinum for the oxygen reduction reaction (ORR) in polymer electrolyte membrane fuel cells. In this work, a copper single atom coordinated by nitrogen doped carbon nanotubes is employed as a support for the deposition of platinum nanoparticles (Pt/Cu-SAC), according to the prediction of the density functional theory calculation, which reveals the ORR activity of Pt/Cu-SAC should be improved in comparison to that of Pt/C due to the weaker adsorption of oxygen. The prepared Pt/Cu-SAC exhibits more promising ORR activity than the commercial Pt/C due to the synergetic effect of Cu-SAC on the Pt particles. Furthermore, the fuel cell based on Pt/Cu-SAC with a cathode Pt loading of 0.025 mg cm–2 exhibits a peak power density of 526 mW cm–2, which is quite similar to that obtained with the commercial Pt/C with a cathode Pt loading of 0.1 mg cm–2. The Pt/Cu-SAC paves the way to design low-Pt cathode catalysts for the polymer electrolyte membrane fuel cells.
研究领域:
材料科学
·
能源科学
·
催化化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）