ChemCatChem
·
2023
·Vol. 15
·期 20
·e202300793
·
IF 4.5
Guoqing Wang,Miao Jiang,Zhao Sun,Leilei Qian,Guangjun Ji,Lei Ma,Cunyao Li,Hong Du,Li Yan,Yunjie Ding
Graphical A multifunctional heterogeneous Pd-POPs-CF 3 SO 3 H catalyst containing integrated acid and metal sites and anions was synthesized for tandem conversion of fructose to bio-diketones in good yield with an extraordinary TOF. Tandem conversion of biomass to value-added fine chemicals is a significant challenge. For instance, the production of fine chemicals from fructose involves conversion to 5-hydroxymethylfurfural (5-HMF), followed by another reaction and purification. Dual catalyst systems have been used in nearly every study on the tandem conversion of fructose to bio-diketones. Therefore, a sole multifunctional heterogeneous catalyst was developed in this study for the tandem conversion of fructose to bio-diketones, which has not been reported previously. Instrument corrosion and the separation or purification of 5-HMF were avoided using the multifunctional heterogeneous catalyst, which contained integrated active sites of acid, metal, and anions. The multifunctional CF 3 SO 3 H-functionalized porous-organic-polymers(POPs)-supported Pd catalyst (Pd-POPs-CF 3 SO 3 H) was prepared using a series of modifications. A bio-diketone yield of 51.0 % was achieved using Pd-POPs-CF 3 SO 3 H in the tandem conversion of fructose with an excellent TOF of 88.3 h −1 which is much more efficient than catalyst reported in literatures. Pd-POPs-CF 3 SO 3 H could be reused at least three times with stable performance. Control experiments and characterization results proved that the high specific surface area, hierarchical pore structure, abundance of CF 3 SO 3 −1 anions, and proximity of Pd moieties and acid sites (“The closer the better” principle) led to the decent performance for bio-diketone.
研究领域:
催化
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化学工程
·
有机化学
·
绿色化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Guangjun Ji,Cunyao Li,Pan Gao,Miao Jiang,Lei Ma,Guoqing Wang,Guangjin Hou,Li Yan,Yunjie Ding
Tuning the microenvironment surrounding single atom metals is an effective but challenging way to regulate the performance of single atom catalysts (SACs). Herein, we prepared a series of P, N-abundant porous organic polymers (P&N-POPs) with diverse framework flexibility and coordination ability to serve as SACs’ carriers. The microenvironment (coordination site, coordination number) surrounding Rh and the equilibrium of ea / ee -HRh(CO) 2 P 2 active species were effectively regulated in Rh/P&N-POPs catalysts. Our study shows that the specific active ee -HRh(CO) 2 (P) 2 species confined in the flexible polymeric skeleton endowed the Rh/ m PPh 3 &PPD-POP with superior activity (TOF = 2000 h −1 ), selectivity of aldehydes (93.5 %), ratio of linear aldehyde to branched aldehyde (l/b ratio = 15.9), favorable stability (10 recycling runs without activity loss) and extensive substrate applicability (19 kinds of olefins) in hydroformylation reactions. Multiple characterization techniques (EXAFS, STEM, in-situ FTIR etc.) were employed to get insights into this effective strategy to regulate the performance of single atom catalysts (SACs).
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Xiang-Cheng Lin,Miaomiao Hu,Minzhe Li,Jian Liu,Qinjie Kou,Rong Huang,Lixian Sun,Changchun Wen
The molecular diagnosis of diseases through the highly sensitive and specific detection of very small amounts of biomarkers in biological samples remains a great challenge, and powerful detection strategies are urgently needed for basic research and clinical applications. Herein, a novel synergistic signal amplification strategy based on Au/Fe 3 O 4 /POPs to integrate magnetic porous composite Fe 3 O 4 /POPs with strong adsorption capabilities for target molecules and gold nanoparticles (AuNPs) with plasmonic properties, is proposed for ultra-high sensitivity and specific Surface-enhanced Raman spectroscopy (SERS) detection of the gastric cancer marker 4-hydroxybenzoic acid (4-HBA). The Au/Fe 3 O 4 /POPs-based SERS assay for gastric cancer-related biomarkers achieved significantly enhanced SERS signals arising from multiple signal amplifications, had good linear calibration from 10 −11 to 10 −5 mol/L, and could detect 4-HBA with a limit of detection (LOD) as low as 1.52 × 10 −12 mol/L. The detection of 4-HBA doped serum exhibited good specificity, homogeneity, and reliability. This material is easy to synthesize and simplifies the sample pretreatment process. This innovative SERS substrate is promising for the rapid detection of disease markers, particularly for early diagnosis and monitoring the effectiveness of gastric cancer treatments.
研究领域:
分析化学
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生物医学
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纳米材料科学
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DOI
高影响因子
Scientific Reports
·
2016
·Vol. 6
·期 1
·1-13
·
IF 5.228
Cagnetta Giovanni,Liu Han,Zhang Kunlun,Huang Jun,Wang Bin,Deng Shubo,Wang Yujue,Yu Gang
Brominated organic pollutants are considered of great concern for their adverse effect on human health and the environment, so an increasing number of such compounds are being classified as persistent organic pollutants (POPs). Mechanochemical destruction is a promising technology for POPs safe disposal because it can achieve their complete carbonization by solvent-free high energy ball milling at room temperature. However, a large amount of co-milling reagent usually is necessary, so a considerable volume of residue is produced. In the present study a different approach to POPs mechanochemical destruction is proposed. Employing stoichiometric quantities of Bi 2 O 3 or La 2 O 3 as co-milling reagent, brominated POPs are selectively and completely converted into their corresponding oxybromides (i.e. BiOBr and LaOBr), which possess very peculiar properties and can be used for some actual and many more potential applications. In this way, bromine is beneficially reused in the final product, while POPs carbon skeleton is safely destroyed to amorphous carbon. Moreover, mechanochemical destruction is employed in a greener and more sustainable manner.
研究领域:
环境科学
·
化学工程
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产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 2
·121635
·
IF 7.5
Shirui Zhao,Zhenxiang Jiang,Yunshuang Hu,Yingzhu Yang,Zhixia Li,Zhaojin Ran,Zhongmin Wang,Yiting Wang,Hua Cen,Guang Deng
There is an urgent need to develop efficient strategies to remove the plant growth regulator forchlorfenuron (CPPU), due to its persistent contamination of aquatic environments. A cost-effective imine-linked porous polymer (Pre-DAP-IPA-POPs) was synthesized through the condensation of 2,6-diaminopyridine (DAP) with isophthalaldehyde (IPA), followed by in situ reduction with KBH 4 to obtain DAP-IPA-POPs. Under optimized conditions (298 K, pH 7, 2 h, and 10 mg of adsorbent), the material achieved a CPPU adsorption capacity of 98.62 ± 8.29 mg·g −1 . Thermodynamic analysis indicated the exothermic nature of the adsorption process ( ΔH 0 =-10.37 kJ·mol −1 ), while kinetic modeling revealed that adsorption reached equilibrium within 2 h and followed a pseudo-second-order kinetic model. 13 C Solid-state NMR and infrared results indicate that the material was successfully synthesized. Furthermore, the successful adsorption of CPPU was evidenced by the emergence of characteristic Cl 2p signals in the XPS spectra of CPPU@DAP-IPA-POPs. Quantum chemical calculations revealed an electron transfer from the HOMO of the unchlorinated phenyl ring in CPPU to the LUMO of DAP-IPA-POPs, which is primarily localized on the C N groups. Noncovalent interaction (NCI) analysis revealed that hydrogen bonding and van der Waals interactions dominated the adsorption process, with steric repulsion exerting a minor opposing effect. These insights collectively demonstrate the promise of DAP-IPA-POPs as a cost-effective and efficient adsorbent for agricultural wastewater remediation.
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高影响因子
Nanoscale
·
2024
·Vol. 16
·期 18
·8931-8940
·
IF 5.8
Rusong Sang,Yezi Hu,Zewen Shen,Guixia Zhao,Junrong Yue,Xiubing Huang
In light of the widespread use of fossil fuels and the resulting environmental pollution, it is crucial to develop efficient photocatalysts for renewable energy applications that utilize visible light. Organic photocatalysts based on β-ketoenamine offer several advantages, including facile preparation, high stability, structural controllability, and excellent photovoltaic properties. However, in previous studies, the synthesis of porous organic polymers (POPs) often involved long, high-temperature processes. In this study, POPs with donor (D)–acceptor (A) structure were constructed by utilizing various branched bridging groups and 2,4,6-triformylphloroglucinol, across multiple temperature gradients. Through adjustments in hydrothermal temperature, we successfully synthesized a series of POPs with varying enol–keto structure ratios. Among these POPs, the dimethoxybenzidine-POPs (DMDPOPs) with methoxy electron-rich branched chains exhibited superior photovoltaic performance, electron transfer rate, and photocatalytic activity compared to the dihydroxybenzidine-POPs (DHDPOPs) with electron-deficient hydroxyl branched chains. Notably, DMDPOP-30 demonstrated outstanding performance, achieving a conversion rate of 98% within 3 h. Additionally, other POPs exhibited favorable conversions (90%), further confirming the feasibility of this synthetic approach. Moreover, the synthesis of DMDPOP-30 was achieved under mild conditions at room temperature, highlighting its significant potential for practical applications.
研究领域:
材料科学
·
化学工程
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光化学
·
催化
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DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 16
·7748-7757
·
IF 3.925
Danling Cheng,Hewen Li,Shipeng Hu,Tao Zhao
The interaction between metal ions and phospholipids plays an essential role in cellular signal transduction, oxidative lipid damage and other biological processes. Herein, we report fluorescence microscopy analysis of the interaction between Zn2+ on planar supported lipid bilayers (SLBs), as model membranes. The results show that Zn2+ interacts with palmitoyl oleoyl phosphatidylserine (POPS), a negatively charged phospholipid, in palmitoyl oleoyl phosphatidylcholine (POPC) SLBs, which leads to significant structural reorganization of the bilayer. Upon Zn2+ binding, the formation of bilayer stacks was observed, which led to the subsequent disruption of the membrane. The kinetics of bilayer stack formation could be described with a characteristic sigmoidal profile and a three-stage mechanism consisting of a lag phase for initial nucleation (formation of stable nuclei), a subsequent exponential phase for growth (growth of nuclei to bilayer stacks) and a final stationary phase was proposed. The lag time reduced in an exponential fashion with increasing Zn2+ concentration and the lag phase could be essentially eliminated in SLBs with high POPS content. Moreover, a linear dependency of the apparent first-order rate constant for bilayer stack growth on Zn2+ concentration was established. Besides, the equilibrium dissociation constants for Zn2+-membrane interaction were calculated and the affinity between Zn2+ and SLBs increased with an increase in the POPS content in the membrane. These results have important implications in general understanding of ion-mediated malformations of cell membranes and cell fusion. Also, this work provides an interesting in vitro system for studying metal ions interacting with biomembranes.
研究领域:
生物物理
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细胞生物学
·
膜科学
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DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Yuting Jiang,Shiying Yang,Manqian Wang,Yichao Xue,Junqin Liu,Yang Li,Dongye Zhao
Hexabromocyclododecane (HBCD) is one of the priority persistent organic pollutants (POPs), yet a cost-effective technology has been lacking for the removal and degradation of HBCD. Zero-valent aluminum (ZVAl) is an excellent electron donor. However, the inert and hydrophilic surface oxide layer impedes the release of the electrons from the core metallic Al, resulting in poor reactivity towards HBCD. In this research, a new type of modified mZVAl particles (AC@mZVAl bm/NaCl ) were prepared through ball milling mZVAl in the presence of activated carbon (AC) and NaCl, and tested for adsorption and reductive degradation of HBCD in water. AC@mZVAl bm/NaCl was characterized with a metallic Al core with newly created reactive surface coated with a thin layer of crushed carbon nanoparticles . AC@mZVAl bm/NaCl was able to rapidly (within 1 h) adsorb HBCD (C 0 = 2 mg L −1 ) and thus effectively enriched HBCD on the carbon surface of AC@mZVAl bm/NaCl . The pre-enriched HBCD was subsequently degraded by the electrons from the core Al, and ∼63.44% of the pre-sorbed HBCD was completely debrominated after 62 h of the contact. A notable time lag (∼12 h) from the onset of the adsorption to the debromination was observed, signifying the importance of the solid-phase mass transfer from the initially adsorbed AC particles to the reactive Al-AC interface. Overall, AC@mZVAl bm/NaCl synergizes the adsorptive properties of AC and the high reactivity of metallic Al, and enables a novel two-step adsorption and reductive degradation process for treating HBCD or likely other POPs.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
PubMed
高影响因子
Polymer Chemistry
·
2021
·Vol. 12
·期 46
·6745-6754
·
IF 5.582
Zhi-Hao Zhang,Shan-Qing Peng,Shumeng Chi,Hanyuan Chen,Lei Fan,Yan Liu,Xiaohua Ma,Mu-Hua Huang
Porous organic polymers (POPs) are a class of promising materials for overcoming environmental and energy issues worldwide. However, their amorphous nature makes structural characterization in the solid state very challenging. In addition, developing facile synthesis methods and applications for POPs with novel structures remain urgent issues requiring improvement. In this work, novel porous organic polymers (named BIT-POPs) with isolated trans-alkene linkages were synthesized via cross-linking bis-norbornene via ring opening metathesis polymerization (ROMP) in an extremely mild and fast manner. Spectral editing approaches, such as 13C-CPMAS, 13C-CPPI, and 13C-CPNQS, relating to solid-state NMR were used to distinguish the overlapping NMR signals of insoluble BIT-POPs, and two-dimensional 1H–13C HETCOR spectra were used. Also, BIT-POP-5 was added to a polysulfone matrix as a porous filler to form a mixed-matrix membrane, which showed a 126% increase in CO2 permeability during gas separation.
研究领域:
材料科学
·
环境科学
·
能源科学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Jiang Meng,Jianyu Han,Zhi Wang,Chunlei Yang,Xiaoning Lu,Jigang Wang
Persistent organic pollutants (POPs) present a substantial environmental challenge due to their enduring nature and adverse effects on human health. The exploration of photocatalysts featuring abundant active sites and appropriate band structures represents a promising approach for harnessing solar energy in photo-self-Fenton reactions for pollutant oxidation. In this investigation, a two-dimensional S-scheme FeOCl/C 3 N 4 heterostructure was fabricated for the degradation of POPs. The coordination between dangling nitrogen atoms in C 3 N 4 and Fe 3+ in FeOCl established a novel pathway for the transfer of photogenerated electrons, thereby prolonging their lifespan by mitigating recombination events. Assessment of the photocatalytic performance using 4-chlorophenol (4-CP) as a model pollutant revealed a 5.4-fold and 40-fold enhancement in degradation rate over FeOCl/C 3 N 4 compared to individual catalysts. Notably, nearly complete mineralization rates were achievable with FeOCl/C 3 N 4 , underscoring its robustness. Mechanistic investigations delineated hydroxyl radicals (•OH) as the primary active species responsible for pollutant degradation.
研究领域:
环境科学
·
材料科学
·
光化学
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产品关联
DOI
高影响因子
Food Analytical Methods
·
2023
·Vol. 16
·期 9
·1477-1486
·
IF 2.9
Liu Lei,Zhao Binyu,Luo Xiaogang,Meng Lingkui,Wu Fengshou
Porous organic polymers (POPs) are a class of materials that combine the properties of both polymers and porosity. They are characterized by their network structure composed of repeating organic units, which form pores or cavities throughout the material. Owing to their unique features including tunable porosity, abundant accessible active sites and synthetically control ability, POPs have been widely employed in the fields of catalysis, adsorption, and biomedicine. The incorporation of porphyrin building units into POPs endows POPs with unique structural characteristics and excellent optical properties. In this work, the aldehyde porphyrin with polyethylene glycol chain was successfully synthesized with good hydrophilicity, which was then reacted with tetrakis(4-aminophenyl) methane to construct the porphyrin-based porous organic polymers. The porphyrin-based POPs was then metallized to yield iron-containing porous organic polymers (Fe-POPs), which could catalyze the transformation of colorless substrate (3,3′,5,5′-tetramethylbenzidine (TMB)) to a blue product (ox-TMB) in the presence of hydrogen peroxide (H 2 O 2 ). Upon the addition of the ascorbic acid (AA) to the aforementioned system, the blue solution faded gradually to colorless. Based on this phenomenon, a rapid and sensitive colorimetric assay for the measurement of H 2 O 2 and AA was developed using Fe-POPs as mimetic enzyme. Fe-POPs was then successfully applied in real samples to detect AA with high accuracy. As a potential peroxidase mimic, Fe-POPs demonstrated the benefits of excellent stability and catalytic efficiency, which presented the promising application in the area of biocatalysis and biosensing. Graphical
研究领域:
材料科学
·
化学生物学
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分析化学
·
生物化学
·
纳米技术
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Rongrong He,Shenzhen Cong,Jing Wang,Jindun Liu,Yatao Zhang
The computational simulation of porous graphene oxide (PGO) indicated that it has great potential for the preparation of gas separation membranes. However, scaling up the manufacture of multilayer, defect-free porous graphene oxide membrane with consistently sized nanopores is extremely challenging. Here, we prepared layer-by-layer CO2-philic Pebax@1657 membranes that were functionalized by o-hydroxyazo-hierarchical porous organic polymers (o-POPs) and PGO. The d-spacing of pristine PGO could be finely regulated through CO2-philic o-POPs to facilitate the permeability of CO2. In addition, the o-POPs exhibit “N2-phobic, CO2-philic” properties with the phenolic hydroxyl and the azo group. The best of the POP-PGO membrane exhibits that the CO2 permeability and ideal selectivity of CO2/N2 are 232.7 Barrer and 80.7, respectively, and it has surpassed the Robeson’s upper bound (2008).
研究领域:
材料科学
·
化学工程
·
环境科学
✓ 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）