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Inorganic and Nano-Metal Chemistry · 2017 · IF 0

Synthesis, crystal structure and magnetic property of a new Co(II) complex based on 4-phenyl pyridine and 5-sulfoisophthalic acid anion

Jiaxing Li,Meng Ni,Chaoyi Fan,Yan Li,Xiuqing Zhang

A new cobalt complex [Co3(SIP)2(4-PP)8(H2O)6]·4H2O·2(4-PP) (1) with 5-sulfoisophthalic acid sodium (NaH2SIP) and 4-phenyl pyridine (4-PP) as ligands has been synthesized in the mixed solvents of ethanol and water. It crystallized in monoclinic, space group P21/c, with a = 20.9642(9) Å, b = 15.6091(5) Å, c = 20.0126(8) Å, α = 90.00°, β = 115.493(6)°, γ = 90.00°, V = 5911.2(4) Å3, Z = 2, Dc = 1.346 g/cm−3, F(000) = 2494, the final GOOF = 1.038, Rint = 0.0258 and wR2 = 0.1793. The complex (1) was characterized by single-crystal X-ray diffraction, magnetic susceptibility and IR spectroscopy analyses. Single-crystal X-ray diffraction shows that complex (1) is trinuclear based on cobalt units. Magnetic susceptibility measurement indicates that complex (1) shows an antiferromagnetic coupling between the Co(II) ions.

研究领域: 无机化学 · 材料科学
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APPLIED CATALYSIS A-GENERAL · 2021 · IF 5.706

Base-free atmospheric O2-mediated oxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic acid triggered by Mg-bearing MTW zeolite supported Au nanoparticles

Lei Chen,Wenxia Zhuang,Jingmin Lan,Xiaoling Liu,Shi Jiang,Lei Wang,Yu Zhou,Jun Wang

Mg-bearing MTW silicalite zeolite, MgSi-ZSM-12, was straightforwardly synthesized by involving an unusual acidic pre-gelation system and engaged as the task-specific support for loading the Au nanoparticles (NPs). The resulting Au/MgSi-ZSM-12 catalyst showed stably excellent activity for the oxidation of HMF into FDCA in the presence of atmospheric dioxygen (O 2 ) without externally adding any liquid base, affording a yield of 87 % and turnover number (TON) of 331 based on the surface Au sites. Superior basicity was evidenced by embedding Mg species into the all-silica zeolitic skeleton, which enables strong, weak, and near-zero affinity towards aldehyde, alcohol, and carboxyl groups, respectively, thus, allows rapid and high-uptake adsorption of HMF, but negligible adsorption of FDCA. This unique feature of the Mg-bearing all-silica zeolite support together with its synergy with the active sites of Au NPs is revealed to accelerate the production of FDCA under the base-free mild condition.

研究领域: 催化化学 · 材料科学 · 环境化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF HAZARDOUS MATERIALS · 2019 · IF 7.65

Effect of calcium addition in plasma catalysis for toluene removal by Ni/ZSM-5 : Acidity/basicity, catalytic activity and reaction mechanism

Weicheng Xu,Bingxu Chen,Xueding Jiang,Feng Xu,Xin Chen,Limin Chen,Junliang Wu,Mingli Fu,Daiqi Ye

The effect of Ca modification on the Ni/ZSM-5 catalyst for efficient toluene oxidation was studied in a plasma-catalytic system. The Ni/ZSM-5 and Ca-Ni/ZSM-5 catalysts were prepared by a wet impregnation method and characterized by X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET), Fourier transform infrared (FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS), Pyridine-FTIR spectroscopy and temperature programmed desorption of ammonia (NH 3 -TPD). Among the catalysts tested, the Ca-Ni/ZSM-5 sample showed the best potential for toluene conversion (90.2%) and CO 2 selectivity (70.7%). Pyridine-FTIR spectra and NH 3 -TPD results proved that the introduction of Ca and Ni onto ZSM-5 caused a decrease in the strong and weak acidic sites. In addition, gas chromatography/mass spectrometry (GC-MS) result showed that the Ca-Ni/ZSM-5 catalyst reduced the production of undesirable byproducts (such as p-nitrotoluene and methyl benzoate). Calcium in the Ni/ZSM-5 system influenced the acidity and other surface characteristic of the catalyst, as well as directly impacting the reactive plasma species and the intermediates. Finally, possible reaction mechanisms in the plasma catalysis of toluene were also proposed.

研究领域: 环境催化 · 大气污染控制 · 材料化学 · 表面科学 · 等离子体化学
✓ 已验证 DOI 高影响因子
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RESEARCH ON CHEMICAL INTERMEDIATES · 2023 ·Vol. 49 ·期 10 ·4523-4539 · IF 3.3

Conversion of glucose into 5-hydroxymethylfurfural by carbonaceous solid acid catalysts loaded with Brønsted acid and Lewis acid in biphasic system

Guo Hui,Han Long,Baloch Humair Ahmed,Wang Zhonghui,Xia Jia,Zhang Chengkun,Yin Xuejian

Biomass-derived 5-Hydroxymethylfurfural (HMF) is a vital platform compound for synthesizing biofuel and various high-value chemicals. This work prepared carbonaceous solid acid catalysts with Brønsted acid and Lewis acid using pine biomass as raw materials through chloride salts impregnation, carbonization and sulfonation. The obtained catalysts were characterized by XRD, FTIR, SEM–EDS, BET, and Py-IR. The catalysts were applied to convert glucose into HMF in a biphasic system involving NaCl solution and γ-valerolactone. The results showed that the catalyst of PC-Al-SO 3 H exhibited larger microspheres and pore sizes compared with the sulfonated catalyst of PC-SO 3 H without AlCl 3 impregnation. Effects of key variables such as reaction temperature, reaction time on conversion of glucose into HMF were examined. By using PC-2Al-SO 3 H with stronger Lewis acid, glucose conversion and HMF yield achieved 86.53 mol% and 59.62 mol% at 160 °C and 6 h. The cyclic experiments revealed that PC-2Al-SO 3 H exhibited relatively stable activity.

研究领域: 生物质化学 · 催化化学
✓ 已验证 DOI 高影响因子
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ANALYTICA CHIMICA ACTA · 2024 · IF 5.7

Rational tuning of binding properties of pillar [5] arene-based sensing material by synergistic effect and its application for fluorescent turn-on detection of isoniazid and controlled reversible morphology

Jian-Peng Hu,Qi Zhao,Qi Lin,Hong Yao,You-Ming Zhang,Tai-Bao Wei

Isoniazid ( INH ) is crucial in the treatment of tuberculosis; however, its overuse may induce significant gastrointestinal and hepatic side effects. On October 27, 2017, the International Agency for Research on Cancer, under the auspices of the World Health Organization, published a list of carcinogens for preliminary collation and reference. Isoniazid was categorized as a Group 3 carcinogen. The efficient detection of INH poses an important and challenging task. In this study, a “synergistic effect” is incorporated into the pillar (Yamagishi and Ogoshi, 2018) [5] arene-based macrocyclic host ( DPA ) by strategically attaching bis-p-hydroxybenzoic acid groups to the opposite ends of the pillar (Yamagishi and Ogoshi, 2018) [5] arene. This combination endows DPA with a reversible and selective fluorescence response to isoniazid. Additionally, DPA exhibits excellent analytical capabilities for isoniazid, including speed and selectivity, with a detection limit as low as 4.85 nM. Concurrently, DPA can self-assemble into a microsphere structure, which is convertible into micrometer-sized tubular structures through host-guest interactions with isoniazid. The introduction of a competitive guest, trimethylamine, enables the reversion to its microsphere structure. Consequently, this study presents an innovative and straightforward synthetic approach for smart materials that facilitates the reversible morphological transition between microspheres and microtubes in response to external chemical stimuli. This discovery provides a valuable strategy for designing “synergistic effects” in constructing trace-level isoniazid-responsive interfaces, with potential applications across various fields, such as controlled drug delivery.

研究领域: 分析化学 · 材料科学 · 药物化学
✓ 已验证 DOI PubMed 高影响因子
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RENEWABLE ENERGY · 2023 · IF 8.7

Renewable biomass-derived, P-doped granular activated carbon for efficient oxidation of 5-hydroxymethylfurfural to 2,5-diformylfuran: Insights into the crucial role of P and N functionality

Zhu Yin,Fengzhen Wu,Changfu He,Lirong Tang,Yandan Chen,Guanfeng Lin,Biao Huang,Jing Chen,Beili Lu

Heteroatom-doped carbon materials for eco-friendly metal-free catalysis have gained increasing attention, but they nevertheless face technological challenges relating to the difficult recycling and high cost. In this work, P-doped granular activated carbons with intrinsic N functionality (PN-GAC-T) were successfully fabricated from low-cost and sustainable waste peanut shells using a simple self-bonding strategy assisted by phosphoric acid. The as-prepared PN-GAC-T were found to have abundant N, P functional groups and large specific surface areas, making them potentially efficient metal-free catalysts for the selective oxidation of 5-hydroxymethylfurfural (HMF). Catalytic results showed that an excellent HMF conversion (98.4%) and 2,5-diformylfuran (DFF) selectivity (99.7%) could be achieved under mild conditions via employing PN-GAC-800 as a catalyst. The good catalytic performance of PN-GAC-800 is highly reliant on the synergistic effect between doped P and intrinsic N functionalities as verified by the control experiments. Furthermore, the density functional theory (DFT) calculations demonstrated that the introduction of both P and N functional groups would aid in the activation of HMF and the improvement of oxygen adsorption capability. This work has emphasized the possibility of high-value exploitation of biomass waste, and it is predicted to provide new inspiration for the development of readily recyclable heteroatom-doped carbon catalysts.

研究领域: 材料科学 · 环境科学 · 催化化学
✓ 已验证 DOI 高影响因子
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Advanced Sustainable Systems · 2021 ·Vol. 5 ·期 6 ·2000297 · IF 6.271

Solvent-Promoted Oxidation of Aromatic Alcohols/Aldehydes to Carboxylic Acids by a Laccase-TEMPO System: Efficient Access to 2,5-Furandicarboxylic Acid and 5-Methyl-2-Pyrazinecarboxylic Acid

Ai-Di Cheng,Min-Hua Zong,Guang-Hui Lu,Ning Li

Laccase coupled with 2,2,6,6-tetramethylpiperidinyl-1-oxy (TEMPO) is a well-known catalytic system for the oxidation of alcohols to the carbonyl compounds. In this work, a simple yet effective solvent engineering strategy is developed to enable aromatic alcohols/aldehydes to be efficiently oxidized to carboxylic acids by a laccase-TEMPO system. Citrate buffer (100–300 m m , pH 6) rather than the widely used acetate buffer (pH 4–5) proves to be optimal for this purpose. The roles of citrate are discussed in laccase-TEMPO-catalyzed synthesis of carboxylic acids. 5-Hydroxymethylfurfural (HMF) of 200 m m is oxidized to 2,5-furandicarboxylic acid (FDCA), a top-value biobased chemical in the polymer industry, in 28 h with a yield of up to 97%. Of the 18 substrates examined, 11 alcohols are converted to target carboxylic acids with >90% yields by this method, with 2 alcohols giving >60% yields of carboxylic acids. Gram-scale preparation of FDCA and 5-methyl-2-pyrazinecarboxylic acid, an important drug intermediate, is demonstrated with total turnover numbers up to 110 000 for laccase and space-time yields up to 1.0 g/(L•h). This chemoenzymatic approach may be a promising alternative to traditional chemical oxidations for the synthesis of carboxylic acids.

研究领域: 生物化学 · 酶工程 · 绿色化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF CHEMICAL RESEARCH · 2021 · IF 0.782

Syntheses, crystal structures, and fluorescent properties of three coordination polymers with 5-sulfoisophthalic acid anion and 4-phenylpyridine

Fangmin Chen,Chichi Zhou,Yan Li,Xiuqing Zhang

Three coordination polymers—{[Ag2(SIP)(4-pp)]·[Ag(4-pp)2]·H2O}n, [Pb4(SIP)2(μ3-OH)2(H2O)2]n, and {[Zn2(SIP)2(4-pp)4][Zn(4-pp)2(H2O)4]·4H2O}n (SIP = 5-sulfoisophthalic acid anion, 4-pp = 4-phenylpyridine)—are constructed under hydrothermal or solvothermal conditions using sodium m-phthalate 5-sulfonate (NaH2SIP) and 4-phenylpyridine as ligands. The structures of the three complexes are determined by single-crystal X-ray diffraction, powder X-ray diffraction, thermogravimetric analyses, Fourier-transform infrared analysis, and photoluminescence. The fluorescent properties of the complexes in the solid state are investigated at room temperature, and the results indicate that they all show photoluminescent properties.

研究领域: 无机化学 · 材料科学 · 晶体学
✓ 已验证 DOI 高影响因子
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES · 2024 ·Vol. 25 ·期 5 ·2693 · IF 4.9

A Glycosyl Hydrolase 5 Family Protein Is Essential for Virulence of Necrotrophic Fungi and Can Suppress Plant Immunity

Xiaofan Liu,Huihui Zhao,Jiatao Xie,Yanping Fu,Bo Li,Xiao Yu,Tao Chen,Yang Lin,Daohong Jiang,Jiasen Cheng

Phytopathogenic fungi normally secrete large amounts of CWDEs to enhance infection of plants. In this study, we identified and characterized a secreted glycosyl hydrolase 5 family member inSclerotinia sclerotiorum(SsGH5,Sclerotinia sclerotiorumGlycosyl Hydrolase 5).SsGH5was significantly upregulated during the early stages of infection. Knocking outSsGH5did not affect the growth and acid production ofS. sclerotiorumbut resulted in decreased glucan utilization and significantly reduced virulence. In addition,Arabidopsis thalianaexpressing SsGH5 became more susceptible to necrotrophic pathogens and basal immune responses were inhibited in these plants. Remarkably, the lost virulence of theΔSsGH5mutants was restored after inoculating ontoSsGH5transgenicArabidopsis. In summary, these results highlight thatS. sclerotiorumsuppresses the immune responses ofArabidopsisthrough secreting SsGH5, and thus exerts full virulence for successful infection.

研究领域: 植物病理学 · 分子生物学 · 微生物学
✓ 已验证 DOI PubMed 高影响因子
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Catalysis Science & Technology · 2025 · IF 4.2

Thermal Switching of Brønsted Acid Sites in Defective UiO-66 Governs the Activity of Fructose Dehydration to 5-Hydroxymethylfurfural

Kai Yan,Zhihao Yu,Yingqing Li,Mengyan Guo,Yuanyu Wang,Xuebin Lu

The efficient dehydration of fructose to 5-hydroxymethylfurfural (HMF) is a crucial step in biomass valorization, requiring solid acids with precisely balanced Brønsted acidity. Defect engineering in Zr-based metal–organic frameworks (MOFs), such as UiO-66, is well known to enhance Lewis acidity; however, its impact on tailoring Brønsted acid sites remains insufficiently understood. Here, we demonstrate that defective UiO-66 possesses a dual-origin Brønsted acid system, comprising intrinsic μ3–OH groups and water molecules coordinated to defect-generated Lewis acidic Zr centers (Zr–H2O). The concentration of these Brønsted acid sites can be finely regulated by thermal activation treatment. A volcano-shaped dependence of catalytic activity on activation temperature is observed, with an optimum at 200 °C. At moderate activation temperatures below 200 °C, the removal of physisorbed water exposes both μ3–OH and Zr–H2O sites, maximizing Brønsted acid density and HMF yield. Activation beyond 200 °C reduces both types of Brønsted acid sites, resulting in diminished catalytic performance. This study reveals the cooperative effect of defect engineering and thermal activation in tuning the Brønsted acidity of MOFs, providing a rational strategy for designing highly selective catalysts for the sustainable production of platform chemicals.

✓ 已验证 产品关联 DOI 高影响因子
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2024 ·Vol. 31 ·期 13 ·19738-19752 · IF 0

Fe-ZSM-5 zeolite catalyst for heterogeneous Fenton oxidation of 1,4-dioxane: effect of Si/Al ratios and contributions of reactive oxygen species

Tian Kun,Pan Jie,Liu Yun,Wang Ping,Zhong Ming,Dong Yuanhua,Wang Meng

Heterogeneous Fenton oxidation using traditional catalysts with H 2 O 2 for the degradation of 1,4-dioxane (1,4-DX) still presents challenge. In this study, we explored the potential of Fe-ZSM-5 zeolites (Fe-zeolite) with three Si/Al ratios (25, 100, 300) as heterogeneous Fenton catalysts for the removal of 1,4-DX from aqueous solution. Fe 2 O 3 or ZSM-5 alone provided ineffective in degrading 1,4-DX when combined with H 2 O 2 . However, the efficient removal of 1,4-DX using H 2 O 2 was observed when Fe 2 O 3 was loaded on ZSM-5. Notably, the Brønsted acid sites of Fe-zeolite played a crucial role during the degradation of 1,4-DX. Fe-zeolites, in combination with H 2 O 2 , effectively removed 1,4-DX via a combination of adsorption and oxidation. Initially, Fe-zeolites demonstrated excellent affinity for 1,4-DX, achieving adsorption equilibrium rapidly in about 10 min, followed by effective catalytic oxidative degradation. Among the Fe-ZSM-5 catalysts, Fe-ZSM-5 (25) exhibited the highest catalytic activity and degraded 1,4-DX the fastest. We identified hydroxyl radicals (·OH) and singlet oxygen ( 1 O 2 ) as the primary reactive oxygen species (ROS) responsible for 1,4-DX degradation, with superoxide anions (HO 2 · /O 2 · − ) mainly converting into 1 O 2 and ·OH. The degradation primarily occurred at the Fe-zeolite interface, with the degradation rate constants proportional to the amount of Brønsted acid sites on the Fe-zeolite. Fe-zeolites were effective over a wide working pH range, with alkaline pH conditions favoring 1,4-DX degradation. Overall, our study provides valuable insights into the selection of suitable catalysts for effective removal of 1,4-DX using a heterogeneous Fenton technology.

研究领域: 环境科学 · 催化化学
✓ 已验证 DOI PubMed
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DALTON TRANSACTIONS · 2016 ·Vol. 46 ·期 1 ·193-199 · IF 4.177

LiRb2LaB2O6: a new rare-earth borate with a MOF-5-like topological structure and a short UV cut-off edge

Dongdong Xu,Fangfang Zhang,Yanzhou Sun,Zhihua Yang,Binghua Lei,Lili Liu,Shilie Pan

A new rare-earth borate LiRb2LaB2O6 (LB-1) has been synthesized using a high-temperature solution method. Interestingly, it shares its topological structure with the famous porous material MOF-5, which is formed from Zn4O(BDC)3 (BDC = 1,4-benzenedicarboxylate). The nodes [OZn4] and organic linkers [BDC] of MOF-5 are carefully substituted with La3+ rare-earth cations and the inorganic linkers [BO3] and [LiO4], respectively, in order to construct a pure inorganic open framework. LB-1 exhibits good thermal and water stability. Moreover, it possesses a short cut-off edge (<190 nm) and moderate birefringence (exp. 0.040@589.5 nm, cal. 0.038@589.5 nm). Further insights into the cut-off edge were given by first-principles calculations. The factors that influence the birefringence of LB-1 were discussed in view of the spatial arrangement of the [BO3] anionic groups.

研究领域: 无机化学 · 材料科学 · 晶体工程 · 光学材料 · 固体化学
✓ 已验证 DOI 高影响因子
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