Materials Today Chemistry
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2022
·
IF 7.613
Tian Xia,Zhuangzhuang Wu,Ying Liang,Wenxin Wang,Yongpeng Li,Zhuyin Sui,Linlin Shan,Chaokun Li,Ruimei Fan,Qi Chen
The design and fabrication of versatile covalent organic frameworks (COFs) with multiple properties for diverse applications is highly desirable. Here, the difunctional COFs material g–C 18 N 3 –COF was prepared and modified to be applied for efficient photocatalytic degradation of Rhodamine B (RhB) and pH detection, respectively. Owing to the triazine unit which was suitable for photocatalyst construction, g–C 18 N 3 –COF was sensitive to visible light and exhibited excellent photocatalysis capability toward RhB. Specially, the photocatalytic degradation of RhB with a high concentration of 300 ppm using g–C 18 N 3 –COF reached equilibrium within 6 h. Moreover, g–C 18 N 3 –COF was further grown in-situ onto the filter paper to generate a novel composite material g–C 18 N 3 –COF@Paper with bright yellow fluorescence. g–C 18 N 3 –COF@Paper could visualize the pH detection by remarkable changes in its fluorescent intensity and color in the range of pH value from 1 to 5, on account of the protonation of the nitrogen atoms from the triazine ring in g–C 18 N 3 –COF. The triazine-based sp 2 carbon-conjugated g–C 18 N 3 –COF, respectively, used as photocatalyst and sensor in this work offers a new strategy to construct the versatile COFs material, facilitating the application of functional COFs in the environmental protection field.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
Nature Chemistry
·
2025
·
IF 20.2
Li Shengxu,Xu Shunqi,Lin En,Wang Tonghai,Yang Haoyong,Han Junyi,Zhao Yuxiang,Xue Qunji,Samorì Paolo,Zhang Zhenjie,Zhang Tao
sp 2 -carbon-linked covalent organic frameworks ( sp 2 c-COFs) are crystalline porous polymers with repeat organic units linked by sp 2 carbons, and have attracted increasing interest due to their robust skeleton and tunable semiconducting properties. Single-crystalline sp 2 c-COFs with well-defined structures can represent an ideal platform for investigating fundamental physics properties and device performance. However, the robust olefin bonds inhibit the reversible-reaction-based crystal self-correction, thus yielding polycrystalline or amorphous polymers. Here we report an imine-to-olefin transformation strategy to form single-crystal sp 2 c-COFs. The isolated single crystals display rectangular nanotube-like domains with sizes up to approximately 24 μm × 0.8 μm × 0.8 μm, and permanent pore distribution around 1.1 nm. The highly conjugated olefin linkage endows the crystals with enhanced electronic connectivity which determines a remarkable room-temperature metal-free ferromagnetism (8.6 × 10 −3 emu g −1 ). Our protocol is robust and generally applicable for the synthesis of single-crystalline sp 2 c-COFs for future spin-electron devices.
研究领域:
材料科学
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化学
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Guoqiang Yu,Yuyang Liu,Xuejie Yang,Yarong Li,Yongqiang Li,Yanbo Zhang,Chiyang He
Synthesis of fully sp 2 -carbon conjugated covalent organic frameworks (COFs) is generally considered extremely challenging due to the low reversibility of the C C bond. Herein, a novel sp 2 -carbon conjugated COF material, named sp 2 c-TFPA-pXD, was prepared by Knoevenagel reaction employing tris(4-formylphenyl)amine with triangular geometry as the knot and p-xylylene dicyanide with symmetric structure as the linker unit. The C C linkages topologically connect the two precursors to a fully sp 2 -carbon conjugated 2D lattice and develop an eclipsed layer framework, giving sp 2 c-TFPA-pXD outstanding stability. The prepared sp 2 c-TFPA-pXD does not decompose in nitrogen atmosphere up to 323 °C, and can be stably present in boiling water, acids, bases and common organic solvents. The excellent chemical and thermal stability of sp 2 c-TFPA-pXD makes it suitable for the harsh environment of radioiodine treatment. In fact, sp 2 c-TFPA-pXD shows moderate iodine capture capacity in iodine vapor (1.22 g/g), and also shows acceptable iodine capture performance under real industrial conditions of high temperatures and low iodine concentrations. The iodide capture properties of sp 2 c-TFPA-pXD can be attributed to its regular channels and sp 2 -carbon conjugate structure. In addition, sp 2 c-TFPA-pXD can be reused by simple ethanol soaking treatment, and can almost maintain its original iodine capture performance after five cycles. In addition, sp 2 c-TFPA-pXD also displays noteworthy capability as adsorbent for iodine in cyclohexane solution. Our study confirms that sp 2 c-TFPA-pXD is an excellent candidate material for capturing iodine from air and solutions in harsh environments. We hope that the report of sp 2 c-TFPA-pXD for iodine capture could open up new avenues for sp 2 -carbon conjugated COFs applications and encourage more research to explore the radioiodine capture potential of other stable COFs.
研究领域:
材料科学
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环境科学
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放射性废物处理
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2023
·
IF 13.6
Ying Zhang,Huilin Liu,Baoguo Sun
A new strategy for nereistoxin-related insecticide, cartap, detection in foodstuff and the environment is of great importance due to its poisoning of human beings through direct exposure or via biomagnification . Herein, a highly planar conjugated sp 2 carbon-connected COF (F-C sp 2 -TT) was synthesized via Knoevenagel condensation reaction followed by the post-modification to develop a new platform for cartap visual detection in agricultural and food samples. The synergistic effect of highly planar conjugation and dense functional groups in the opened framework endowed F-C sp 2 -TT with a high-precision luminescence sensing performance. Meanwhile, the exquisitely designed F-C sp 2 -TT presented robust chemical stability, radiation stability, and good reproducibility. Benefiting from these advantages, high-precision luminescent F-C sp 2 -TT achieves a low detection limit of 0.51 μg/L to cartap over the range of 1–300 μg/L ( R 2 =0.9938), and the recoveries percentage in food products was calculated as 95.90%− 119.3%. More significantly, the smartphone-based high-precision platform by F-C sp 2 -TT was established and successfully applied to portable monitoring of cartap and water content. Therefore, our work revealed the enormous potential of C sp 2 -connected COF, which opened a new situation for insecticide detection.
研究领域:
材料科学
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分析化学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Solar RRL
·
2025
·
IF 4.7
Ziyang Jia,Yang Lu,Wenyan Li,Yiyi Fan,Yawen Tang,Lei Cheng,Hanjun Sun
Covalent organic frameworks (COFs), are promising candidates for photoelectrochemical hydrogen evolution reaction (PEC HER). In this study, sp 2 -c COF photocathodes were synthesized on copper foam via Knoevenagel condensation polymerization, with the crystallinity systematically tuned by varying reaction conditions. By modulation, the alkalinity of the reaction system, crystallinity-related parameters were optimized, revealing significant variations in the structural integrity of the resulting sp 2 -c COFS. Under optimal synthesis conditions (110°C, 30 μL pyridine, 2 days), the photocathode demonstrated a photocurrent density of 60 μA cm −2 at 0.3 V versus RHE, a value 2.5 times higher than that observed for samples with suboptimal crystallinity. These results emphasize the positive impact of increased crystallinity in improving PEC HER performance and provide insights for scalable photocathode design.
研究领域:
材料化学
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物理化学
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能源科学
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纳米材料
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电化学
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产品关联
DOI
高影响因子
Materials
·
2018
·Vol. 11
·期 7
·1199
·
IF 2.467
Ling Wang,Yan Zhang,Yongqiang Yang,Jing Zhang
Graphene and its derivatives have been demonstrated to be good surface-enhanced Raman scattering (SERS) substrates. However, the literature offers some contrasting views on the SERS effect of graphene-based materials. Thus, understanding the mechanism of the SERS enhancement of graphene is essential for exploring its application as a SERS substrate. In this study, graphene oxide (GO) and chemically reduced graphene oxide (CRGO) films with different morphologies and structures were prepared and applied as SERS substrates to detect Raman dye molecules. The observed enhancement factors can be as large as 10~103. The mechanism of SERS enhancement is discussed. It is shown that the SERS effect was independent of the adsorption of dye molecules and the surface morphologies of graphene-based films. Raman shifts are observed and are almost the same on different graphene-based films, indicating the existence of charge transfer between dye molecules and substrates. The Raman enhancement factors and sensitivities of dye molecules on different films are consistently within theIG/IDratios of graphene-based substrates, indicating that the dramatically enhanced Raman spectra on graphene-based films are strongly dependent on the average size ofsp2carbon domain.Keywords:graphene oxide;graphene;surface-enhanced Raman scattering (SERS);oxygen-containing groups;chemical enhancement;sp2carbon domain
研究领域:
材料科学
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光谱学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yanan Shang,Xinning Liu,Yanwei Li,Yue Gao,Baoyu Gao,Xing Xu,Qinyan Yue
The synthesis of a highly efficient and stable single atom catalyst (SAC) for peroxydisulfate (PDS) activation remains a challenge. Herein, a reconstructed iron single atom catalyst (Fe-SAC) with both abundant conjugated π-π sp 2 structured carbon and reactive Fe-N 4 sites was first reported to improve the decomposition of organics in PDS/SACs systems. Enhanced organics adsorption can be achieved by the conjugated π-π sp 2 structured carbon via π-π interaction to decrease the migration distance of reactive species to organic molecules. In addition, PDS tended to be attached onto the Fe-N 4 sites accompanied by the peroxymonosulfate (PMS) generation via S-O breakage of PDS, accelerating the generation of radicals. As a result, organics decomposition via PDS activation by reconstructed Fe-SAC was significantly higher (∼6 times) than the conventional Fe-SAC because of the synergistic effect of the resulting dual reaction sites. This work provides a new strategy to enhance the catalytic performances in PDS/SACs systems.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
Analytical Methods
·
2022
·Vol. 14
·期 24
·2389-2395
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IF 3.532
Jia You,Qianqian Kong,Cuiling Zhang,Yuezhong Xian
A new fully conjugated covalent organic framework material (COFTFPPy–ThDAN) has been synthesized via the Knoevenagel condensation reaction using 1,3,6,8-tetra(4-formylphenyl)pyrene (TFPPy) as the chromogenic unit and 2,2′-([2,2′-bithiophene]-5,5′-diyl)diacetonitrile (ThDAN) as the linker. The COFTFPPy–ThDAN has been successfully prepared under the optimized conditions and showed excellent crystallinity and chemical stability. Especially, it was able to maintain its crystallinity even when immersed under harsh conditions such as HCl (3 M) and NaOH (3 M). Meanwhile, COFTFPPy–ThDAN exhibited good fluorescence properties, which could remain relatively stable under different pH conditions. Moreover, COFTFPPy–ThDAN was further employed for the detection of Fe3+ with high sensitivity and selectivity with a limit of detection (LOD) of 1.26 μM. COFTFPPy–ThDAN with high stability and fluorescence is a promising material for chemical sensing.
研究领域:
材料科学
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分析化学
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化学传感
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Lisha Liang,Yuxiang Zhao,Wuxin Zhang,Haokai Yan,Mengwei Chen,Yuan Chen,Jin Zhou,Tao Zhang
The sp 2 -carbon-conjugated porous polymers (sp 2 c-CPPs) that possess high porosity, chemical stability, and carrier mobility are potential for uranium extraction from seawater, which is tremendous meaningful for the rapidly growing demands of the nuclear industry due to the abundant uranium resources (4.5 billion tons) in ocean. Here, we report the synthesis of three sp 2 c-CPP films (DMPN-TFPT, BN-TFPT and TMTN-TFPT) directly on Cu substrate that can work as electrodes for electrochemical uranium extraction. Furthermore, we designed a photovoltaic-electrocatalysis (PV-EC) system to enhance the uranium extraction capacity, meanwhile, modified oxime groups on sp 2 c-CPPs film to enhance uranium ion selectivity. The DMPN-TFPT electrode shows ultra-high uranium extraction performance (1022.02 mg m −2 ) in 8 ppm uranyl-spiked simulated seawater, which is higher than that of BN-TFPT film (426.27 mg m −2 ) and TMTN-TFPT film (607.30 mg m −2 ) because of the higher in-plane electron delocalization. Additionally, in ultra-low concentration of simulated seawater (3.3 ppb), the DMPN-TFPT film also exhibited a high capacity up to 81.74 mg m −2 within 30 days. This work shows the great potential of sp 2 c-CPP films on solar-driven electrochemical uranium extraction.
研究领域:
材料科学
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环境工程
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核工程
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电化学
·
太阳能
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产品关联
DOI
高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2023
·Vol. 120
·期 14
·e2219043120
·
IF 11.1
Huan Wang,Youzeng Li,Maoyu Wang,Shan Chen,Meng Yao,Jialei Chen,Xuelong Liao,Yiwen Zhang,Xuan Lu,Edward Matios,Jianmin Luo,Wei Zhang,Zhenxing Feng,Jichen Dong,Yunqi Liu,Weiyang Li
Despite the various strategies for achieving metal–nitrogen–carbon (M–N–C) single-atom catalysts (SACs) with different microenvironments for electrochemical carbon dioxide reduction reaction (CO2RR), the synthesis–structure–performance correlation remains elusive due to the lack of well-controlled synthetic approaches. Here, we employed Ni nanoparticles as starting materials for the direct synthesis of nickel (Ni) SACs in one spot through harvesting the interaction between metallic Ni and N atoms in the precursor during the chemical vapor deposition growth of hierarchical N-doped graphene fibers. By combining with first-principle calculations, we found that the Ni-N configuration is closely correlated to the N contents in the precursor, in which the acetonitrile with a high N/C ratio favors the formation of Ni-N3, while the pyridine with a low N/C ratio is more likely to promote the evolution of Ni-N2. Moreover, we revealed that the presence of N favors the formation of H-terminated edge of sp2 carbon and consequently leads to the formation of graphene fibers consisting of vertically stacked graphene flakes, instead of the traditional growth of carbon nanotubes on Ni nanoparticles. With a high capability in balancing the *COOH formation and *CO desorption, the as-prepared hierarchical N-doped graphene nanofibers with Ni-N3 sites exhibit a superior CO2RR performance compared to that with Ni-N2 and Ni-N4 ones.
研究领域:
材料科学
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电化学
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催化
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纳米技术
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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）