Environmental Science-Nano
·
2023
·Vol. 10
·期 11
·3072-3083
·
IF 7.3
Chuanqi Pan,Biluan Zhang,Tingyu Pan,Hui Huang,Siyi Song,Xitong Cai,Yuhang Wang,Hongwei Sun,Zhu Luo,Lizhi Zhang,Yanbing Guo
The dual activation mechanism of molecular oxygen (O2) and water (H2O) in the local structure of catalysts has not been elucidated yet. Herein, we report a strategy for manufacturing fully exposed Ag4 sites in nano silver/graphdiyne (Ag/GDY) composites for activating O2 and H2O. The synthesized nano Ag was uniformly anchored on the surface of GDY without any surfactant added, with an average particle size of 2.5 nm. The unique sp-hybrid C and triangular pore structure of GDY not only regulate the stable geometric structure of nano Ag, but also enhance the adsorption ability of Ag4 sites for O2 and H2O molecules in nano Ag/GDY. Electron spin resonance spectroscopy and density functional theory calculation results proved that O2 is more favorable to synergistically promote the activation of H2O to generate reactive ·O2− and ·OH radicals on the nano Ag/GDY surfaces, leading to outstanding antibacterial activity. This work provides a simple strategy for the preparation of stable nano Ag and proposes to improve the catalytic oxidation activity by adjusting the local electronic structure of catalysts to activate O2 and H2O.
研究领域:
材料科学
·
催化化学
·
微生物学
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产品关联
DOI
高影响因子
AQUATIC TOXICOLOGY
·
2025
·
IF 4.3
Wei Hong,Fan Zhang,Zhuang Wang
Graphdiyne (GDY), an emerging 2D carbon nanomaterial, holds promise yet remains unexplored for environmental hazards. Herein, we investigated the toxicity effects and mechanisms of GDY towards the freshwater microalga Scenedesmus obliquus at environmentally relevant concentrations. The results revealed that 1 mg/L of GDY inhibited the growth of the algae and significantly induced a decrease in photosynthetic pigments. Exposure to 0.1 and 1 mg/L of GDY led to a reduction in cell membrane permeability and induced intracellular oxidative stress in the algae. Further, 1 mg/L of GDY caused oxidative damage to the algal cells. Molecular modeling indicated that GDY could directly affect the stability of dsDNA fragment. Transcriptome analysis showed that GDY at 1 mg/L influenced the expression of 2216 genes, with the glycerolipid metabolism pathway being enriched significantly. Metabolome analysis identified 129 differentially expressed metabolites (DEMs) in the algae exposed to 1 mg/L of GDY, revealing three significantly disrupted pathways: glycerophospholipid metabolism, pentose phosphate pathway, and flavonoid biosynthesis. The integrated transcriptome and metabolome analysis suggested that GDY exposure downregulated the level of a lysophosphatidylcholine species (LPC 18:3) by inhibiting the expression of genes related to FMN binding molecular functions. Simultaneously, the algae responded to GDY exposure by upregulating genes involved in the biological process of carbohydrate metabolic process and the molecular function of hydrolase activity, as well as increasing the levels of DEMs, specifically a lysophosphatidic acid species (LPA 16:4). This study elucidates the stress mechanisms induced by GDY in aquatic organisms and emphasizes the importance of monitoring its acute biological effects.
研究领域:
环境科学
·
分子生物学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Ying Zhang,Rui Zhu,Jiang Zhong,Zhipeng Quan,Yongjian Zhu,Jingling Yang,Ping Liang,Jin Yong Lee,Hongguang Liu
Transition-metal-atom anchored graphdiynes (TM@GDY, TM = Mn, Fe, Co, Ni and Cu) have already been synthesized and found applications in hydrogen evolution , nitrogen fixation and etc. By means of first-principle predictions and test experiments, we propose here that Fe@GDY and Co@GDY are efficient catalysts for the sustainable conversion of O 3 to O 2 . These two catalysts can spontaneously chemisorb O 3 with zero reaction barrier and have low O 3 conversion barriers (0.31 eV and 0.19 eV, respectively). The O 3 decomposition experiment in a continuous flow membrane reactor and electron paramagnetic resonance results verify that Fe@GDY and Co@GDY are efficient catalysts under humid conditions. Raman spectra prove the formation of the key Fe-O/Co-O and Fe O O and Co O O intermediates. The hydrophobic nature of graphdiyne and the strongest chemisorption of O 3 among tested ambient gases, make Fe@GDY and Co@GDY ideal catalysts under both dry and humid conditions. These findings would stimulate future explorations on metal anchored GDY-based catalysts for applications of toxic gas decomposition or fixation.
研究领域:
材料科学
·
环境科学
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产品关联
DOI
PubMed
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2025
·Vol. 27
·期 8
·4278-4289
·
IF 2.9
Ziyu Li,Mei Li,Rongsheng Xu,Zhiliang Jin
The electron transfer rate in photocatalysts is one of the factors determining their hydrogen production activity. In this work, NH2-MIL-88B(Fe) (NFM) was synthesized using a one-step hydrothermal synthesis method and NFM/GDY-25 (NFMG-25) was successfully synthesized by loading graphdiyne (GDY) onto the surface of NFM. The hydrogen production performance and the mechanism of the prepared photocatalysts were systematically investigated using XRD, SEM, FT-IR, XPS, UV-Vis, PL and photoelectrochemical tests. The results showed that the hydrogen production of NFMG-25 reached 61.7 μmol in 5 hours. Photoelectrochemical and Mott–Schottky tests demonstrated that the composite catalyst exhibited high photogenerated carrier separation efficiency and single catalysts were n-type semiconductors. The conduction bands of NFM and GDY were −0.36 V and −0.56 V, respectively, while the valence bands were 1.90 V and 1.12 V. NFM acted as an electron acceptor and donor, which accelerated the transfer of the electrons, and enhanced the photocatalytic hydrogen production efficiency of the composite system. This study provides an effective method for using NFM in photocatalytic hydrogen production.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Jianing Wang,Haokai Yan,Yuxiang Zhao,Daheng Wu,Haoyong Yang,Xiaodong Yin,Runxiang Tan,Tao Zhang
Copper-based materials are very important for many application fields from marine industry to energy management and electronic devices. For most of these applications, the copper objects require long-term contact to a wet and salty environment, which leads to serious corrosion of copper. In this work, we report a thin graphdiyne layer directly grown on arbitrary shapes of copper objects at mild conditions, which could function as a protective coating for the copper substrates in artificial seawater with corrosion inhibition efficiency of ∼99.75%. To further improve the protective performance of the coating, the graphdiyne layer is fluorinated and followed by infusion with a fluorine-containing lubricant (i.e., perfluoropolyether). As a result, a slippery surface is obtained, which shows enhanced corrosion inhibition efficiency of ∼99.99% as well as excellent antibiofouling properties against microorganisms, such as protein and algae. Finally, the coatings are successfully applied in the protection of a commercial copper radiator from long-term attack of artificial seawater without disturbing its thermal conductivity. These results demonstrate the great potential of graphdiyne-based functional coatings for the protection of copper devices in aggressive environments.
研究领域:
材料科学
·
化学工程
·
海洋科学
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Yanqing Wang,Jianjiang He,Zengqi Zhang,Zhihong Liu,Changshui Huang,Yongcheng Jin
Graphdiyne (GDY), a new type of carbon material with an electron-rich conjugated structure, has been investigated as a separator coating layer to enhance the electrochemical performance of lithium–sulfur (Li–S) battery. Acetylenic bond (−C≡C–C≡C−) and benzene ring in the GDY coating layer are experimentally verified to reversibly attract the soluble lithium polysulfides by chemical adsorption during cycling. Meanwhile, the shuttle effect of soluble polysulfides is further physically restricted by the GDY coating layer due to the evenly distributed pores (5.42 Å) and a consistent interlayer spacing (3.65 Å) of GDY. Moreover, GDY is a conducting carbon skeleton with high Li+ mobility that can improve the rate performance. Hence, Li–S battery with an as-prepared GDY coating layer shows excellent electrochemical performances including superior specific capacity, excellent rate performance, and low capacity attenuation rate. The high initial discharge capacity of 1648.5 mA h g–1 at 0.1C and 819.5 mA h g–1 even at a high rate of 2C is achieved by this novel separator. The initial capacity of 1112.9 mA h g–1 at 0.5C is retained to 816.7 mA h g–1 after 200 cycles with a low attenuation rate of 0.13% per cycle. Compared with other coated separators, these results show that the GDY coating layer endows the separator with superior electrochemical performances for Li–S battery.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Tian Wang,Zhiliang Jin
The design and construction of photocatalysts are the crucial step for solar-driven hydrogen evolution. Herein, a new type of graphdiyne (C n H 2n-2 )-based photocatalyst, which was prepared by one pot method, was used to promote hydrogen evolution reaction by constructing GDY/VS 2 ohmic junction with S sites anchoring on the surface. Actually, the unique two-dimensional conjugated carbon network of GDY can maintain the structural stability. The uneven surface facilitates the flow of electrons, which makes GDY a good electron donor. In addition, the expanded interlayer spacing of VS 2 exposes more hydrogen evolution active sites. The increase in surface electronegativity of composite catalysts enhances their redox ability and charge transfer kinetics. The band edge of the graphdiyne-metal sulfide Ohmic contact interface is bent, allowing electrons to flow into the co catalyst without resistance. These synergistic effects lead to the robust hydrogen production of GDY/VS 2 , which was increased by nearly 10.3 times compared with that of pure GDY. Finally, charge migration at the interface of graphdiyne-metal sulfide heterojunction was proposed and further verified combining in situ XPS and theory calculation. This research marks a significant stride for enhance the efficiency of photocatalytic hydrogen evolution by designing and constructing composite heterojunction materials.
研究领域:
材料科学
·
能源科学
·
化学
✓ 已验证
DOI
高影响因子
Small
·
2021
·Vol. 17
·期 38
·2102066
·
IF 13.281
Qian Chang,Fan Wang,Zicheng Zuo,Feng He,Yao Zhao,Fuyi Wang,Yuliang Li
Suppressing the irreversible interfacial reactions is an important scientific bottleneck in the development of stable high-energy-density lithium-ion battery. The interfacial chemistry of graphdiyne (GDY) on the high-voltage cathode of LiNi 0.5 Mn 1.5 O 4 (LNMO) shows a very interesting process, in which the sp-hybridization carbon atoms chemically scavenge the hydrofluoric acid (HF) and in situ form the fluorinated GDY interface. It first turns the harmful HF into profit, and greatly enhances the interfacial stability and restrains the side reaction on the cathode under high working voltage. The GDY-coated LNMO cathode obviously alleviates the electrolyte degradation, achieves high Coulombic efficiency and reliability. Due to atomic-level selectivity and chemical trapping of HF by GDY, it effectively suppresses the dissolution of Mn, Ni elements. These results highlight the unparalleled advantages of GDY in the formation of high stable interfaces and protection of high-energy-density electrodes.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Ziyu Li,Jiqiao Zhang,Mei Li,Meijuan Ding,Zhenkun Liu,Zhiliang Jin
Cost-effective bimetallic oxide catalysts are gradually replacing noble metal catalysts for photocatalytic hydrogen production . This study used a two-step method to synthesize CoMoO 4 with a rod-shaped structurea. CuBr is a catalytic base synthesis graphdiyne material. The graphdiyne that serves to anchor CoMoO 4 rods through a solvent-thermal synthesis method, thereby enhancing the photocatalytic performance of the resultant composite catalyst. The results show that the 5 h hydrogen evolution capacity of the optimized CoMoO 4 /graphdiyne composite catalyst is 187.47 μmol, which is 2.9 times higher than that of CoMoO 4 monomer and 41.7 times higher than that of graphdiyne monomer. The addition of graphdiyne provides a larger comparison area for CoMoO 4 , giving composite catalyst more active sites, and enhancing the optical hydrogenation effect of catalysts. Through the Mott-Schottky test, the UV–visible diffuse reflectance test and band gap calculation can be speculated that the CoMoO 4 and graphdiyne construct the type II heterojunction which promotes the rapid transfer of photogonic carriers. This work provides a good prospect and opportunity for studying graphdiyne in the application of graphdiyne in the application of dualmetal oxides.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2021
·Vol. 413
·期 15
·3847-3859
·
IF 4.157
Xiao Jing,Liu Zhang,Li Chunxiang,Wang Jinglun,Huang Haowen,Yi Qingfeng,Deng Keqin,Li Xiaofang
Graphdiyne (GDY) adsorbed DNA probes have been used as a fluorescent sensing platform, but topics including DNA adsorption affinities, DNA probe displacement, and fluorescence quenching ability were rarely researched. Herein, the adsorption affinity of single-stranded DNA (ssDNA) and double-stranded DNA (dsDNA) on a tremella-like GDY was tuned by modulating the surface chemistry of GDY. The fluorescence quenching ability of GDY with different oxidation degrees was compared. The nonspecific displacement of DNA probes on GDY was studied. Under the same concentrations, GDY with low oxidation degree exhibited stronger adsorption affinity and higher adsorption capacity to both ssDNA and dsDNA than highly oxidized GDY. DNA adsorbed on low-oxidized GDY was more resistant to displacement by other DNAs. Protein showed strong interaction with different GDY and could displace DNA probes on GDY. Based on these findings, an ideal GDY with proper oxidation degree, exhibiting high surface affinity for ssDNA and low affinity for dsDNA, was used as scavenger of redundant ssDNA fluorescent probe in an enzyme-assisted amplification system for sensitive ochratoxin (OTA) detection. This study has enhanced our fundamental understanding of DNA adsorption by GDY. It also provided a rational way to apply GDY for fluorescence sensing in a complicated system. Graphical abstract
研究领域:
材料科学
·
生物化学
·
分析化学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Jiaming Liu,Xiaomei Shen,Didar Baimanov,Liming Wang,Yating Xiao,Huibiao Liu,Yuliang Li,Xingfa Gao,Yuliang Zhao,Chunying Chen
Graphdiyne (GDY) is a novel two-dimensional (2D) carbon allotrope with sp-hybridized carbon atoms and hexagonal rings. Because of its unique structure and electronic property, GDY was reported as a promising candidate applied in energy storage, catalysis, biosensing and so on. However, using GDY as a platform to immobilize metal ion or enzyme was still not reported. Here, we presented a GDY-based composite with dual-enzyme activity by immobilizing ferrous ion and glucose oxidase onto GDY sheet. GDY showed great adsorption capacity and maintained the high catalytic activity of ferrous ion. The ferrous ion preferred to adsorb in between the neighboring two C–C triple bonds of GDY with lower adsorption energy (−5.64 eV) if compared to graphene (−1.69 eV). Meanwhile, GDY exhibited the ability of adsorbing glucose oxidase while did not obviously influence the structure and catalytic activity of the enzyme. The as-prepared composite was successfully used in one-step blood glucose detection. This work provides a new insight on ion and enzyme immobilization by 2D material.
研究领域:
材料科学
·
生物化学
·
医学诊断
✓ 已验证
DOI
PubMed
高影响因子
ChemSusChem
·
2024
·
IF 7.5
Min Cui,Yanan Yuan,Yue Wu,Zhongmei Che,Peixuan Li,Xiaochen Yang,Yuqi Chen,Wei Hu,Jingui Wang,Shuai Wang,Yingshu Guo,Zexing Wu
Graphical This graphical abstract visually summarizes the main findings of the study, showcasing how the strategic design of a GDY-induced CoN/CoS 2 heterojunction within a nitrogen-doped carbon substrate leads to a more efficient and durable electrocatalyst for both oxygen reduction and evolution reactions in high-performance zinc-air batteries. The performance of zinc-air battery is constrained by the sluggish rate of oxygen electrode reaction, particularly under high current discharge conditions where the kinetic process of the oxygen reduction reaction (ORR) decelerates significantly. To address this challenge, we present a novel phase transition strategy that facilitates the creation of a heteroatom-doped heterointerface (CoN/CoS 2 ). The meticulously engineered CoN/CoS 2 /NC electrocatalyst displays a superior ORR half-wave potential of 0.87 V and an OER overpotential of 320 mV at 10 mA cm −2 . Experimental and computational analysis confirm that the CoN/CoS 2 heterostructure optimizes local charge distribution, accelerates electron transfer, and tunes active sites for enhanced catalysis. Notably, this heterojunction improves stability by resisting corrosion and degradation under harsh alkaline conditions, thus demonstrating superior performance and longevity in a custom-made liquid zinc-air battery. This research provides valuable practical and theoretical foundations for designing efficient heterointerfaces in electrocatalysis applications.
研究领域:
材料科学
·
电化学
·
能源存储与转换
✓ 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）