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Green Chemical Engineering 2021年第2期2卷 217-223页

作者： Xian-Tai Zhou Hong-Bing Ji Fine Chemical Industry Research Institute Sun Yat-sen UniversityGuangzhou510275China School of Chemical Engineering Guangdong University of Petrochemical TechnologyMaoming525000China

Substrate specificity is a hallmark of enzymatic *** this work,the biomimetic catalytic oxidation of styrene and cyclohexanone by iron(III)porphyrins and molecular oxygen was carried out,and remarkable differences in efficiency were *** specificity of the substrates for biomimetic catalytic oxidation was investigated by kinetics and mechanistic *** studies revealed that the oxidation of styrene followed Michaelis-Menten kinetics with KM=8.99 mol L^(-1),but the oxidation of cyclohexanone followed first-order kinetics with kobs=1.46×10^(-4) s^(-1),indicating that the styrene epoxidation by metalloporphyrins exhibited characteristics of enzyme-like catalysis,while the oxidation of cyclohexanone was in agreement with the general rules of chemical *** catalytic mechanisms for the two substrates were discussed by operando electron paramagnetic resonance spectroscopy,operando UV-vis spectroscopy,and KI/starch *** specificity was concluded to be attributed to the stability of high-valence species and oxygen transfer rate.

关键词： Substrate specificity Kinetics Oxidation metalloporphyrins Mechanism

Selective oxidation of o-nitrotoluene to o-nitrobenzaldehyde with metalloporphyrins as biomimetic catalysts

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Frontiers of Chemical Science and Engineering 2009年第4期3卷 453-456页

作者： Xinling WANG Yuanbin SHE Institute of Green Chemistry and Fine Chemicals Beijing University of TechnologyBeijing 100124China

Selective oxidation of o-nitrotoluene to onitrobenzaldehyde with metalloporphyrins as biomimetic catalysts was *** peripheral substituent around porphyrin rings and various process parameters of NaOH concentration,reaction temperature,reaction time and oxygen pressure all affect the selectivity of ***,82.0%selectivity of onitrobenzaldehyde was achieved under the optimum conditions:1.0×10^(-5)mol·L^(-1)of T(p-NO_(2))PPFeCl catalyst,2.5 mol·L^(-1)of NaOH,0.2 mol·L^(-1)of o-nitrotoluene,45℃and 2.0 MPa for 6 h.

关键词： o-nitrotoluene o-nitrobenzaldehyde metalloporphyrins

Selective epoxidation of linear terminal olefins with metalloporphyrins under mild conditions

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Frontiers of Chemical Science and Engineering 2009年第3期3卷 310-313页

作者： Xiaoguang BAI Yuanbin SHE Institute of Green Chemistry and Fine Chemicals Department of Chemistry and Chemical EngineeringCollege of Environmental and Energy EngineeringBeijing University of TechnologyBeijing 100124China

The epoxidation of linear terminal olefins with metalloporphyrins in the presence of dioxygen and isobutyraldehyde under ambient temperature and atmo-spheric pressure was *** results show that all olefins could be smoothly converted to epoxides with high selectivities(70%–90%).For the metalloporphyrins with different catalytic activities within 1-hexene epoxidation in the order of Fe>Mn>Co,T(o-Cl)PPFe(III)Cl was most effective,with a 41.7%yield and 80.2%selectivity of 1,*** amounts of catalyst were investi-gated,and it was found that with only 10ppm catalyst the yield of 1,2-epoxyhexane and turnover number(TON)could reach up to 41.9%and 41859,respectively.

关键词： metalloporphyrins olefins dioxygen epox-idation

Electrocatalysis of metalloporphyrins(Ⅷ)——Electrocatalytic Reduction of Molecular Oxygen with Water-Soluble Cobalt (Ⅱ) Tetrakis(4-Trimethyl Ammonium Phenyl) Porphyrin Catalyst

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Chemical Research in Chinese Universities 1990年第2期6卷 102-109页

作者： Wang Zongli, Zhang Hui and Pang Daiwen (Department of Chemistry, Wuhan University , Wuhan)

Reported here is the electrocatalytic reduction of molecular oxygen in the presence of water-soluble cobalt(Ⅱ) tetrakis(4-trimethyl ammonium phenyl) porphyrin (Co(Ⅱ)TTAPP) as catalyst in solutions of various pH values. The overpotential of molecular oxygen reduction is reduced by ca. 200-400 mV in acidic and neutral solutions compared with several decades of millivolts in alkaline solutions, indicating that Co(Ⅱ)TTAPP possesses much higher catalytic activity in acidic and neutral solutions than in alkaline. H2TTAPP in solutions of various pH exhibits no significant catalytic activity for oxygen reduction. The significant difference in the electrocatalytic activity of Co(Ⅱ)TTAPP from that of H2TTAPP for oxygen reduction indicates that the electrocatalytic activity of Co(Ⅱ)TTAPP should be attributed to the central cobalt atom (Co(Ⅱ)) coordinated by N4 internal ring in Co(Ⅱ)TTAPP. The total number of electrons involved in oxygen reduction electrocatalyzed by Co (Ⅱ)TTAPP is 2, and the product of such reaction is H2O2 or HO2-in solutions of various pH. The reaction mechanism of oxygen reduction in acidic and alkaline solutions is also discussed.

关键词： Electrocatalysis metalloporphyrins Electrocatalytic reduction

Analysis of vibrational spectra of nano-bio molecules: Application to metalloporphrins

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Chinese Physics B 2013年第9期22卷 225-232页

作者： K Srinivasa Rao G Srinivas J.Vijayasekhar V.U.M.Rao Y.Srinivas K.Sunil Babu V.Sunndadara Siva Kumar A.Hanumaiah Department of Electronics & Instrumentation Engineering Lakireddy Bali Reddy College of Engineering Department of Physics KL University Research Scholar Department of MathematicsJawaharlal Nehru Technological University Department of Applied Mathematics College of Science & TechnologyAndhra University Department of Computer Science GITAM University Department of Physics Miracle Engineering College Department of Electronics & Instrumentation Rajeev Gandhi Memorial Engineering College Department of Physics Lara's Vignan Institute of Technology and Science

In this paper, we have applied the Lie algebraic model to nano-bio molecules to determine the vibrational spectra of different stretching and bending vibrational modes. The determined vibrational energy levels by the Lie algebraic model are compared with the experimental data. The results from the theoretical mode[ are consistent with the experimental data. The vibrational energy levels are clustering in the excited states.

关键词： Lie algebraic model vibrational spectra vibrational modes metalloporphyrins

Co anchored on porphyrinic triazine-based frameworks with excellent biocompatibility for conversion of CO_(2)in H_(2)-mediated microbial electrosynthesis

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Frontiers of Chemical Science and Engineering 2022年第12期16卷 1761-1771页

作者： Folin Liu Shaohua Feng Siyuan Xiu Bin Yang Yang Hou Lecheng Lei Zhongjian Li College of Chemical and Biological Engineering Key Laboratory of Biomass Chemical Engineering of Ministry of EducationZhejiang UniversityHangzhou 310027China Institute of Zhejiang University—Quzhou Quzhou 324000China Academy of Ecological Civilization Zhejiang UniversityHangzhou 310027China

Microbial electrosynthesis is a promising alternative to directly convert CO_(2)into long-chain compounds by coupling inorganic electrocatalysis with biosynthetic ***,problems arose that the conventional electrocatalysts for hydrogen evolution may produce extensive by-products of reactive oxygen species and cause severe metal leaching,both of which induce strong toxicity toward ***,poor stability of electrocatalysts cannot be qualified for long-term *** problems may result in poor biocompatibility between electrocatalysts and *** solve the bottleneck problem,Co anchored on porphyrinic triazine-based frameworks was synthesized as the electrocatalyst for hydrogen evolution and further coupled with Cupriavidus necator *** showed high selectivity for a four-electron pathway of oxygen reduction reaction and low production of reactive oxygen species,owing to the synergistic effect of Co–Nx modulating the charge distribution and adsorption energy of ***,low metal leaching and excellent stability were observed,which may be attributed to low content of Co and the stabilizing effect of ***,the electrocatalyst exhibited excellent ***,the microbial electrosynthesis system equipped with the electrocatalyst successfully converted CO_(2)to poly-β-*** work drew up a novel strategy for enhancing the biocompatibility of electrocatalysts in microbial electrosynthesis system.

关键词： microbial electrosynthesis hydrogen evolution reaction metalloporphyrins biocompatibility CO_(2)conversion

Manganese porphyrin-mediated aerobic epoxidation of propylene with isoprene: A new strategy for simultaneously preparing propylene epoxide and isoprene monoxide

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Chinese Chemical Letters 2023年第3期34卷 236-239页

作者： Xian-Tai Zhou Hai-Yang Yu Yang Li Hai-Bo Wu Hong-Bing Ji Fine Chemical Industry Research Institute School of Chemical Engineering and TechnologySun Yat-sen UniversityZhuhai 519082China Fine Chemical Industry Research Institute School of ChemistrySun Yat-sen UniversityGuangzhou 510275China Huizhou Research Institute Sun Yat-sen UniversityHuizhou 516081China Advanced Energy Science and Technology Guangdong Laboratory Huizhou 516003China

The direct epoxidation of propylene by O_(2) is a significant and challenging topic. The key factor for this homogeneous aerobic epoxidation is the activation of molecular oxygen under mild conditions. In this work,the aerobic epoxidation of propylene catalyzed by manganese porphyrins was achieved in the presence of isoprene. Isoprene contains an allyl methyl group, and the α-H can be easily removed to achieve the activation of molecular oxygen. The conversion of propylene was 38% and the selectivity toward propylene oxide(PO) was up to 87%. The role of isoprene was demonstrated, and a plausible mechanism was proposed. The protocol reported herein is expected to provide a strategy for the simultaneous preparation of propylene oxide and isoprene monoxide.

关键词： Propylene Epoxidation Dioxygen Isoprene metalloporphyrins

Highly Efficient Oxidative Cleavage of Carbon-Carbon Double Bond over meso-Tetraphenyl Cobalt Porphyrin Catalyst in the Presence of Molecular Oxygen

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Chinese Journal of Chemistry 2012年第9期30卷 2103-2108页

作者：周贤太纪红兵 School of Chemistry and Chemical Engineering Key Laboratory of Low-Carbon Chemistry&EnergyConservation of Guangdong ProvinceSun Yat-sen UniversityGuangzhouGuangdong 510275China

Highly efficient and selective carbon-carbon double bond aerobic cleavage of olefins catalyzed by metallopor- phyrins was investigated, and carbonyl compounds and epoxide were produced as the main products. CoTPP （co- balt meso-tetraphenyl porphyrin） showed excellent activity for the oxidative cleavage of carbon-carbon double bond by using styrene as model compound, in which the TOF （turnover frequency） and selectivity toward benzaldehyde was obtained with 2×10^4h-1 and 86%,respectively.

关键词： oxidative cleavage metalloporphyrins molecular oxygen carbon-carbon double bond

Synthesis of Metal Porphyrins Tailed with Salicylic Acid and their Interaction with Bovine Serum Albumin

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Chinese Chemical Letters 2004年第3期15卷 357-360页

作者： TaoJIA KaiWANG YiMeiZHAO ZaoYingLI DepartmentofChemistry WuhanUniversityWuhan430072 InstituteofRHKCo. Ltd.Wuhan430070

A synthetic method of porphyrins tailed with salicylic substituents is described. Reaction of bromoalkoxyphenyl porphyrin 1 with salicylic acid gave porphyrins 2~5. These new compounds were confirmed by 1H NMR, IR, UV-vis, MS and elemental analysis, and observed their interaction with bovine serum albumin (BSA) in fluorescence spectrum.

关键词： metalloporphyrins salicylic acid synthesis bovine serum albumin fluorescence.

Improvements in SOD mimic AEOL-10150, a potent broad-spectrum antioxidant

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Military Medical Research 2019年第1期6卷 78-88页

作者： Xiao-rui Zhang Wen-xia Zhou Yong-xiang Zhang State Key Laboratory of Toxicology and Medical Countermeasures Beijing Institute of Pharmacology and Toxicology

AEOL-10150 is a broad-spectrum metalloporphyrin superoxidase dismutase(SOD) mimic specifically designed to neutralize reactive oxygen and nitrogen species. Research has shown that AEOL-10150 is a potent medical countermeasure against national security threats including sulfur mustard(SM), nerve agent exposure and radiation pneumonitis following a radiological/nuclear incident sufficient to cause acute radiation syndrome(ARS). AEOL-10150 performed well in animal safety studies, and two completed phase 1 safety studies in patients demonstrated that the drug was safe and well tolerated, indicating that AEOL-10150 has potential as a new catalytic antioxidant drug. In this article, we review improvements in AEOL-10150 in preclinical pharmacodynamic studies, especially regarding anti-SM,chlorine gas and radiation exposure studies.

关键词： Catalytic antioxidant metalloporphyrins Chemical warfare agent Radiation damage Pharmacodynamics Pharmacokinetics