ACS Catalysis
·
2023
·
IF 12.9
Chao Zhang,Yingqiang Li,Yue Xie,Zhanjiang Yu,Xin Wan,Xinzhi Wang,Jiaan He,Junlang Li,Zhenguo Chen,Xiaoyong Li,Xiaohui Yi,Zhaoli Wang,Guang-Guo Ying,Dionysios D. Dionysiou,Mingzhi Huang
Selective hydrodehalogenation and hydrodearomatization of toxic chlorophenols into value-added chemicals represents a grand challenge for their efficient reutilization. For this purpose, single-atom catalysts (SACs) could be a strategy with relatively high catalytic selectivity and atom utilization but suffer from the catalytic limitation caused by low metal loading densities. Graphdiyne and γ-graphyne are considered promising substrates of SACs with excellent catalytic properties. Additionally, their quantum dots with nanometer size are expected to supply numerous surface anchoring sites and large atom spacing to confine metal cations to synthesize high-loading SACs. Here we report a synthesis approach for high-loading Ru SACs anchored on graphdiyne/γ-graphyne quantum dots (GDQD-Ru/GNQD-Ru), which exhibit remarkably higher turnover frequency (TOF) and selectivity (>99%) of hydrodehalogenation and hydrodearomatization of chlorophenols than graphdiyne/γ-graphyne nanosheet-based Ru SACs and nanoparticles. There is no significant selectivity decrease in chlorophenol transformation by GDQD-Ru/GNQD-Ru observed in 5 catalyst reuse cycles. GDQD-Ru/GNQD-Ru contribute to nearly exclusive hydrodehalogenation and hydrodearomatization without altering any other bonds in chlorophenols. Experimental results and theoretical calculations reveal that GDQD-Ru is more prone to lower energies of rate-limiting steps in H2-driven chlorophenol transformation than GNQD-Ru. The results confirm that graphdiyne/γ-graphyne quantum dots play crucial roles in facilitating the metal atom loading of SACs. Ru loadings are 27.6 and 16.0 wt % in GDQD-Ru/GNQD-Ru, approximately 7-fold and 4-fold higher than reported Ru SACs, respectively. This study provides mechanistic insights toward the roles of high-loading Ru SACs on sp- and sp2-hybridized carbonaceous substrates in selective hydrodehalogenation and hydrodearomatization.
研究领域:
化学
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催化科学
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环境科学
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产品关联
DOI
高影响因子
RARE METALS
·
2024
·Vol. 43
·期 4
·1747-1757
·
IF 9.6
Jiang Ming-Ji,Zhang Ya-Na,Meng Ling-Shen,Kang Jing,Li Yong-Jun,Dong Alideertu
Based on the in-situ self-reduction and chemical stability, graphdiyne (GDY) and graphdiyne oxide (GDYO) are used as trapping agents to investigate the ability for recovering Au 3+ , Ag + , and Pd 2+ under different pH values and interfering ions. Under strong acidity at pH = 1, these two agents demonstrate high select recovery towards the three precious metal ions, which could be in-situ reduced to nanoparticles (NPs). In addition, superparamagnetic Fe 3 O 4 NPs are deposited on the surfaces of GDY and GDYO. The magnetic responses enable GDY-Fe 3 O 4 to recover precious metals conveniently and efficiently by the aid of an external magnetic field. This study also confirms the antibacterial activity of the as-recovered NPs deposited on GDY and GDYO against Escherichia coli and Staphylococcus aureus (1 × 10 5 colony-forming unit (CFU)·ml −1 ) , and the antibacterial rates are 100%. This strategy of recovering precious metals and subsequently reusing to combat pathogens will be of great significance for environmental remediation and biomedical applications. Graphical abstract
研究领域:
材料科学
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环境修复
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纳米技术
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生物医学应用
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化学工程
✓ 已验证
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Ying Li,Huan Huang,Rongli Cui,Dongmei Wang,Zi Yin,Dan Wang,Lirong Zheng,Jing Zhang,Yidong Zhao,Hui Yuan,Jinquan Dong,Xihong Guo,Baoyun Sun
In this work, graphdiyne, a new kind of carbon allotrope composed of sp and sp 2 hybridized carbon atoms, firstly worked as an effective electrochemical sensor for the determination of low concentration of Cd 2+ and Pb 2+ in water using electrochemical pre-enrichment and anodic-stripping voltammetry methods. The limit of detection was 0.46 nM for Cd 2+ and 1.72 nM for Pb 2+ with a linear range extended from 0.01 μM to 1 μM. This graphdiyne modified electrode also presented excellent selectivity, stability, applicability and reproducibility, providing a simple and promising platform to develop novel electrochemical sensor for detecting Pb 2+ and Cd 2+ with higher performance. Through X-ray photoelectron spectroscopy (XPS), Fourier-transform infrared (FTIR) and X-ray absorption near edge structure (XANES) characterization, it was verified that the acetylenic links in graphdiyne served as adsorbent sites by providing electrons to bind with heavy metal ions, which enhanced the electrochemical sensing performance.
研究领域:
分析化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
Chemosensors
·
2022
·Vol. 10
·期 11
·485
·
IF 4.229
Yu Zhang,Zhi Xia,Guofeng Gui,Ping Zhang,Qianzhu Li,Lifen Meng
This work constructed an ultrasensitive electrochemical bisphenol AF (BPAF) sensor using ultra-stable graphdiyne-templated platinum nanoparticles (PtNPs@GDY) as a sensing platform. PtNPs@GDY nanocomposite was synthesized by a chemical reduction method, and the preparation process was simple and rapid. GDY, with its natural porous structure, was used as substrate to stabilize PtNPs. Due to the high adsorption ability of GDY, it can prevent PtNPs from aggregation and inactivation. Transmission electron microscopy (TEM), high-resolution TEM (HRTEM) and Energy-dispersive X-ray spectroscopy (EDS) were used to characterize the microstructure and morphologies of the materials. Cyclic voltammetry (CV), Electrochemical impedance spectroscopy (EIS) and differential pulse voltammetry (DPV) were employed to investigate the electrochemical properties of the material and the performance of the sensor. At an optimized condition, the sensor exhibited excellent catalytic activities towards BPAF. The linear ranges were from 0.4 to 15.4 μM and 35.4 to 775.4 μM. The limit of detection was 0.09 μM. In addition, the electrochemical sensor showed good reproducibility, stability and anti-interference.Keywords:graphdiyne;platinum nanoparticles;electrochemical determination;bisphenol AF
研究领域:
材料科学
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环境科学
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分析化学
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产品关联
DOI
高影响因子
MICROCHIMICA ACTA
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2024
·Vol. 191
·期 5
·1-9
·
IF 5.3
Li Yunpeng,Shi Zhuanzhuan,Wu Xiaoshuai,Miao Wenting,Yang Zhengyi,Lou Xinyu,Sun Wei,Guo Chunxian,Li Chang Ming
PEDOT:PSS has been used as a biomimetic uric acid (UA) sensor but suffers from unfortunate low detection limit (LOD), narrow detection range and poor stability. Herein, we get graphdiyne (GDY) marry PEDOT:PSS to create a very stable GDY@PEDOT:PSS heterostructure for a biomimetic UA sensor, which accomplishes the lowest LOD (6 nM), the widest detection range (0.03 μM-7 mM) and the longest stability (98.1% for 35 days) among the related UA sensors. The sensor was successfully used to in situ real-time detection of UA in sweat. The enhancement mechanisms of the sensor were investigated, and results discover that C≡C of GDY and C = C of PEDOT:PSS can cross-link each other by π–π interactions, making not only the former strongly resistant against oxidation deterioration, but also causes the latter to efficiently prevent water swelling of polymer for poor conductivity, thereby leading to high stability from both components. While the stabilized heterostructure can also offer more active sites by enhanced absorption of UA via π-π interactions for highly sensitive detection of UA. This work holds great promise for a practical sweat UA sensor while providing scientific insight to design a stable and electrocatalytically active structure from two unstable components. Graphical abstract
研究领域:
材料科学
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生物医学工程
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分析化学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Peiqi Luo,Liping Wang,Lixia Jiang,Jie Sun,Yafeng Li,Huihui Liu,Caiqiao Xiong,Zongxiu Nie
Graphdiyne (GD) is a new kind of carbon nanomaterial which has carbon–carbon triple bonds to form a layered structure. Here, we report the application of GD as the matrix for small molecule analysis in laser desorption ionization mass spectrometry (LDI MS). The GD matrix displayed two advantages: little background in the low mass range and good molecular ion signal in negative ion mode for many small molecules, e.g., fatty acids, amino acids, peptides, and drugs can be obtained in negative ion mode. By comparing the signal intensity of tetraphenylborate and juglone with and without GD existing, it was found that GD can enhance both of the desorption efficiency and ionization efficiency in LDI. Through analysis of the serum samples from liver cancer patients and healthy people, the GD-assisted LDI MS results showed that fatty acids could be used as potential biomarkers for the early diagnosis of liver cancer.
研究领域:
分析化学
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医学
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产品关联
DOI
PubMed
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Shiguan Xu,Lijun Yan,Hui Cheng,Hui Xie,Lina Zeng,Lin Li,Shuhai He,Wei Sun
In this paper an electrochemical sensor was fabricated by dropping a graphdiyne (GDY) and hemin suspension solution on the surface of carbon ionic liquid electrode (CILE) followed by casting the Nafion film (Nafion/hemin-GDY/CILE). The morphology of GDY was observed by scanning electron microscopy with the biomolecular structure of hemin-GDY and hemin characterized by UV-Vis absorption spectrophotometry, which proved that hemin maintained the original structure after mixing with GDY. Direct electrochemistry of hemin on the GDY modified electrode was realized with a pair of well-defined redox peaks and electrochemical performances were checked in detail with the electrochemical parameters calculated. Nafion/hemin-GDY/CILE showed excellent electrocatalytic ability towards the reduction of bromate with the detection range from 5.00 to 50.0 mmol L -1 and the detection limit of 3.3 mmol L -1 (3 σ ). In addition, the modified electrode possessed good reproducibility and stability, which was applied to the analysis of seawater samples.
研究领域:
分析化学
·
电化学传感器
✓ 已验证
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2023
·
IF 4.5
Haifeng Yao,Yahui Zhang,Yongping Dong,Mingfu Ye
Graphdiyne (GDY) is considered as another promising carbon material in biosensing field. However, the application of GDY in ECL sensing is in its infancy stage, and different roles of GDY are urgent to be discovered. In this work, strong anodic Ru(bpy) 3 2+ electrochemiluminescence (ECL) was obtained at a cucurbit[8]uril (Q[8]) modified electrode. Although GDY exhibited electrocatalytic effect on the oxidation of Ru(bpy) 3 2+ , an apparent inhibiting effect of GDY on the ECL signal was observed due to the energy transfer. An “on-off-on” mode ECL sensor was fabricated to detect pancuronium (PMD) based on the competitive host–guest interaction between ferrocene (Fc), PMD and Q[8]. Fc modified single-stranded DNA was immobilized onto the surface of GDY, which could be attached onto the electrode through the interaction between Fc and Q[8]. The quenching effect of GDY could apparently decrease ECL signal. PMD exhibited stronger combining ability with Q[8] than Fc, and could replace Fc from the cavity of Q[8], leading to the recovery of ECL signal. The variation of ECL intensity changed linearly with the PMD concentration in the range of 10 nM to 50 μM with a detection limit of 5 nM (3σ). The proposed sensor has high sensitivity, outstanding specificity and accuracy, indicating that GDY has promising potential application in ECL sensing field based on its inhibiting effect.
研究领域:
分析化学
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生物传感
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材料科学
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产品关联
DOI
高影响因子
DIAMOND AND RELATED MATERIALS
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2024
·
IF 4.3
Zixiang Hao,Yang Chen,Linrui Wang,Yuxuan Lu,Chengli He,Mingyan Wang,Xiaoli Cui
Elemental engineering has been employed to adjust molecular framework and electronic configuration of γ-graphyne for rapid lithium storage. Here, we construct a quasi-pyridinic nitrogen/sulfur co-doped γ-graphyne (N/S-GY) via a mechanochemical strategy and reveal its lithium storage behavior by quantitative kinetics analysis and theoretical calculations. The internal pyridinic-N atoms create rhombic channels for Li + passing through, while sulfur dopants anchored with alkynyl groups induce electron cloud rearrangement to facilitate intralayer Li + diffuse between C 12 -triangular channels and interlayer transfer through open rhombic channels. As a result, the as-prepared N/S-GY exhibits a high reversible capacity of 1003 mAh g −1 at 50 mA g −1 after 150 cycles, with Li + diffusion coefficient up to 2.6 × 10 −12 cm 2 s −1 , both of which are larger than that of N-doped γ-graphyne. This work highlights synergistic effect of sulfur and nitrogen co-doping in alkynyl carbon and inspires bottom-up heteroatom modification in framework design.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
ADVANCED MATERIALS
·
2020
·Vol. 32
·期 23
·2001082
·
IF 27.398
Ye Zhang,Pu Huang,Jia Guo,Rongchao Shi,Weichun Huang,Zhe Shi,Leiming Wu,Feng Zhang,Lingfeng Gao,Chao Li,Xiuwen Zhang,Jialiang Xu,Han Zhang
Graphdiyne (GDY), a newly emerging 2D carbon allotrope, has been widely explored in various fields owing to its outstanding electronic properties such as the intrinsic bandgap and high carrier mobility. Herein, GDY-based photoelectrochemical-type photodetection is realized by spin-coating ultrathin GDY nanosheets onto flexible poly(ethylene terephthalate) (PET) substrates. The GDY-based photodetectors (PDs) demonstrate excellent photo-responsive behaviors with high photocurrent ( P ph , 5.98 µA cm - 2 ), photoresponsivity ( R ph , 1086.96 µA W - 1 ), detectivity (7.31 × 10 10 Jones), and excellent long-term stability (more than 1 month). More importantly, the PDs maintain an excellent P ph after 1000 cycles of bending (4.45 µA cm - 2 ) and twisting (3.85 µA cm - 2 ), thanks to the great flexibility of the GDY structure that is compatible with the flexible PET substrate. Density functional theory (DFT) calculations are adopted to explore the electronic characteristics of GDY, which provides evidence for the performance enhancement of GDY in alkaline electrolyte. In this way, the GDY-based flexible PDs can enrich the fundamental study of GDY and pave the way for the exploration of GDY heterojunction-based photodetection.
研究领域:
材料科学
·
电子工程
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理论计算
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产品关联
DOI
PubMed
高影响因子
ENERGY & FUELS
·
2024
·
IF 5.2
Yupu Sun,Shengjun Luo,Rongbo Guo
Considering the high thermal conductivity of metal nanofluids and carbon-based nanomaterials as well as the promoting effect of surfactant on hydrate formation, in this study, first, graphyne was coated on the surface of CuNW by in situ growth, and then the surface of intermediate CuNW@GDY was modified with sulfonate ion by emulsion polymerization to obtain the final product CuNW@GDY-PSS, which was used in the methane hydrate experiments. The morphology of synthesized CuNW@GDY-PSS was confirmed by SEM and TEM, and it has a transparent wrinkled structure. In methane hydrate formation experiments, compared with CuNW@GDY, CuNW@GDY-PSS can shorten the induction time by 74.8%, from 45.37 ± 4.83 to 11.42 ± 1.41 min. Furthermore, the experimental results indicate that CuNW@GDY-PSS obtained when the mass ratio of CuNW@GDY to sulfonic acid ions is 0.4 has the best promoting effect on the hydrate experiments. In addition, CuNW@GDY-PSS has good hydrophilicity and good cycling in the multicycle methane hydrate formation and dissociation experiments, which would have potential applications for natural gas storage and transportation.
研究领域:
材料科学
·
化学工程
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Pan Yang,Jinlan Tang,Zhuorui Ding,Yiqun Chen,Zizheng Liu,Jianping Yuan,Yuhua Zhu,Pengchao Xie
Carbocatalysts, widely regarded as eco-friendly catalysts in the field of peroxymonosulfate (PMS) activation for pollutant removal, exhibit significant variations in performance depending on the type of carbon atom hybridization. Notably, the novel graphdiyne (GDY), characterized by its sp-hybridized carbon (sp-C), has recently garnered significant attention. However, the precise mechanistic role of sp-C on PMS activation remains unclear. Herein, we elucidate the role of sp-C on PMS activation and the corresponding mechanism behind enhanced phenolic pollutant degradation over the GDY catalyst. GDY demonstrates exceptional phenolic removal efficiency (97 %), which far exceeds that of traditional sp 2 -hybridized graphene (2 %). The GDY facilitates pollutant oxidation via a catalyst-mediated electron transfer mechanism. The sp-C provides additional sites for PMS adsorption and donates significantly more electrons from GDY to PMS (0.51 e more than graphene), effectively facilitating PMS activation, intermediate species conversion, and reaction kinetics during phenolic pollutant degradation. By integrating the monolithic GDY catalyst into a flow-through device for continuous phenolic pollutant removal, long-lasting phenolic removal was maintained for over 80 hours, with a removal rate exceeding 85 %. This work highlights that sp-C in GDY effectively enhances PMS activation, providing a pathway for efficient organic pollutant degradation in advanced oxidation processes.
研究领域:
环境科学
·
催化化学
✓ 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）