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INORGANIC CHEMISTRY COMMUNICATIONS · 2024 · IF 4.4

Cu-NADH as laccase mimics for efficient aryl C-H amination

Xuyong Tang,Fengxi Li,Sijun Huang,Li Xu,Lei Wang,Yi Guo

Nicotinamide-adenine dinucleotide (NADH) as biomimetic units combined with copper ion to form laccases mimics (Cu-NADH). Cu-NADH has the enhanced activity of copper center to mediate aryl C–H amination using air as green oxidants. It could successfully catalyze oxidative coupling between different aromatic compounds and 4-phenylurazole (yield: 72 ∼ 91 %). Recycling catalytic ability (up to 6 times) showed its excellent stability. The Cu-NADH nanozyme was certificated to catalyze C–H amination effectively, and highlighted that it was a proper way to design catalysts according to enzyme-like catalyzing non-natural reaction.

CAS / MDL: 15988-11-1
研究领域: 生物化学 · 催化化学 · 环境科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2016 · IF 8.328

A bio-inspired strategy to enhance the photocatalytic performance of g-C3N4 under solar irradiation by axial coordination with hemin

Xia Chen,Wangyang Lu,Tiefeng Xu,Nan Li,Dandan Qin,Zhexin Zhu,Gangqiang Wang,Wenxing Chen

In nature, metalloporphyrins, such as chlorophyll, cytochrome P450 and so forth, are key materials in maintaining the ecological cycles, especially the carbon cycle, and play an important role in both photosynthesis and the catalytic oxidation of organisms. Inspired by these factors, we skillfully combined photocatalysis and biomimetic catalysis using imidazole (IMD)-functionalized modification of g-C 3 N 4 and axial coordination with hemin. Compared with pure hemin, g-C 3 N 4 and a mixture of the two, our novel catalytic system (g-C 3 N 4 -IMD-hemin/H 2 O 2 ) showed high photocatalytic oxidation activity for the degradation of 4-chlorophenol (4-CP), and the stability of hemin was enhanced under solar irradiation. Furthermore, the effect of pH and the sustained photocatalytic oxidation stability of g-C 3 N 4 -IMD-hemin for degrading 4-CP were investigated. The results indicated that g-C 3 N 4 -IMD-hemin presents a high photocatalytic oxidation activity over a wide pH range and exhibits good recyclability. A series of designed experiments showed that superoxide radicals ( O 2 − ), high-valent iron (Fe(IV)   =   O) species, peroxy radicals ( OOH) and few hydroxyl radicals ( OH) were generated in the g-C 3 N 4 -IMD-hemin/H 2 O 2 system. This synergistic photocatalytic and biomimetic process offers new insight for the utilization of solar energy and offers a new perspective for the exploration of catalysts for environmental remediation.

研究领域: 环境科学 · 生物化学 · 材料科学
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CHEMICAL ENGINEERING RESEARCH & DESIGN · 2022 · IF 4.119

A catalytic membrane based on dopamine directional deposition biomimetically induced by immobilized enzyme for dye degradation

Shuyan Ma,Chenjie Wei,Hong Jiang,Zhili Chen,Zhikang Xu,Xiaojun Huang

Dopamine-assisted deposition technology is widely used in functional modification of polymer membranes due to the advantages such as simple operation, mild reaction, and strong adhesion to materials. Limited by the major defects of spontaneous polymerization in an alkaline environment and non-selective adhesion, it is still challenging to achieve directional deposition, stability, and fast deposition rate at the same time. Herein, inspired by tyrosinase-induced melanin directional deposition on the skin, we present a biomimetic catalysis strategy for the directional deposition of dopamine on the target surface. By immobilizing laccase on the target surface, the oxidative self-polymerization of dopamine can be inhibited, and the biomimetic induced directional deposition on membrane can be achieved. The biomimetic catalytic membrane covered with a uniform and stable laccase-dopamine coating can be used for the degradation of azo printing and dyeing wastewater. Moreover, the degradation efficiency of the catalytic membrane for methyl orange can reach 19.8 μg/min, and the relative activity can still be maintained at about 81% after 6 cycles, showing high catalytic activity and stability.

CAS / MDL: 2580-56-5 2783-94-0
研究领域: 环境科学 · 生物化学 · 材料科学
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Small · 2025 · IF 12.1

Engineering Atomic Sites and Proton Transfer Microenvironments for Bioinspired Photocatalytic Alcohol-Amine Coupling

Huimin Yi,Chenyi Wang,Baoxin Ge,Fangjie Xu,Pengyang Jiang,Min Zhou,Fangshu Xing,Caijin Huang

Achieving a precise understanding and accurate design of heterogeneous catalysts based on bioinspired principles is challenging yet crucial to digging out optimal materials for artificial catalysis. Here, an ADH-mimicking dual-site photocatalyst (YCuCdS) is developed, and demonstrates the powerful effects of atomic site configuration and proton transfer environments on alcohol-amine coupling. Mechanism studies reveal that the alcohol substrate is effectively dehydrogenated at the Y sites, forming the carbonyl intermediates that rapidly experience condensation with the amine. Meanwhile, the released hydrogen species (H ads ) migrate from adjacent Cu sites to active S atoms, promoting H 2 production and hindering the over-hydrogenation of imine. As a result, a high imine yield of 92% is achieved, along with an H 2 production rate of 7400 µmol g −1 h −1 . This work showcases an effective strategy for the design of heterogeneous catalysts with bioinspiration.

研究领域: 化学工程 · 生物化学 · 材料科学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2013 · IF 2.206

Enhancement of Catalytic Activities of a Biomimetic Catalyst FePz(dtnCl2)4 for the Wet Oxidation of Brilliant Red X3B through the Synergetic Effect of Heat and Light Irradiation

Zehui Zhang,Qiaoli Peng,Jie Sun,Liping Fang,Kejian Deng

In this study, catalytic wet oxidation of Reactive Brilliant Red X3B (abbreviated as X3B) was studied using hydrogen peroxide as oxidant in the presence of a biomimic catalyst, iron(II) tetra(5,6-dichloro-1,4-dithiin)porphyrazine [abbreviated as FePz(dtnCl2)4]. Important factors including the solution pH, H2O2 concentration, and reaction temperature were investigated in detail to optimize the catalytic activity for the removal of X3B. Under the optimal conditions, X3B was degraded by 97.0% at pH = 2 for 240 min. Activation energy and rate constants at different reaction temperatures were calculated for the degradation of X3B in both the dark reaction and photoreaction. These results demonstrated that the catalytic activities of FePz(dtnCl2)4 for the wet oxidation of X3B could be efficiently enhanced through the synergetic effect of heat and light irradiation. Through fluorescence technology, hydroxyl radical (HO•) was detected as the main reactive oxidative species for the oxidative degradation of X3B.

研究领域: 环境科学 · 催化化学
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Coatings · 2024 ·Vol. 14 ·期 4 ·453 · IF 2.9

Cu/Mn Synergy Catalysis-Based Colorimetric Sensor for Visual Detection of Hydroquinone

Ningning Xing,Lilin Yang,Li Wang,Yanxiang Lu,Hongkun Zhang,Xijun Sun,Min Zhao,Wenjie Tan,Jie Yang

The reliable detection of environmental contaminants can correctly forecast the degree of environmental pollution that has occurred, which contributes to improving the environmental purification rate and maintaining the ecological balance. Herein, a novel hierarchical biomimetic catalysis MnO2@CuAl-CLDHs was designed and synthesized using a facile method, which exhibited significantly enhanced peroxidase-like activity due to the unique composition and hierarchical mesoporous structure. Under optimized operational conditions, a visible colorimetric array based on the superior nanozyme activity of MnO2@CuAl-CLDHs was developed for the quantitative determination of hydroquinone with a wide linear detection range (1–100 μM) and a low detection limit (0.183 μM). Simultaneously, our presented strategy could analyze hydroquinone in real water samples with high accuracy. Therefore, the bimetallic co-catalyzed nanozymes are expected to be the perfect replacement for natural enzymes to develop convenient and efficient sensors.

研究领域: 环境科学 · 生物化学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2020 · IF 3.99

Investigating the properties of nano core-shell CeO2@C as haloperoxidase mimicry catalyst for antifouling applications

Nan Wang,Wangqiang Li,Yadong Ren,Jizhou Duan,Xiaofan Zhai,Fang Guan,Lifei Wang,Baorong Hou

Developing environmental and cost-effective antifouling technologies is essential to solve serious biofouling problems. Recently, enzyme mimics and halogenating enzymes have caught progressively attention as valuable tools to combat biofilm formation. In this work, the core-shell structure of CeO 2 @C, as one effective haloperoxidase-like enzyme mimics, was successfully synthesized using the carbon sphere as template through a simple coprecipitation method. Through the UV–vis absorption spectra and kinetic measurements, the CeO 2 @C displays intrinsic haloperoxidase-like activity via catalyzing the bromination of organic signaling compounds. Meanwhile, the prepared CeO 2 @C catalyst process high catalytic stability and recyclability, corresponding to a well catalytic performance repeatability after refresh of raw substrates (at least 10 times). The antibactrial property of CeO 2 @C as haloperoxidase mimicry is evaluated by immersing titanium plate/CeO 2 @C modified titanium plates into bacterial suspensions with different conditions for 4 h at 37 °C. It can catalyze the oxidation of Br − with H 2 O 2 to the corresponding hypobromous acid (HBrO), which exhibits strong antibacterial activity against Gram-negative ( Escherichia coli ), Gram-positive ( Staphylococcus aureus ) bacteria and typical marine ( Pseudomonas aeruginosa ) bacteria. This study introduces a stable, non-poisonous and inexpensive biomimetic material for antibacterial, antifouling and disinfection applications based on novel sustainable and conservation methods.

CAS / MDL: 10294-41-4
研究领域: 生物化学 · 材料科学 · 环境科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2019 · IF 14.229

Construction of biomimetic catalysis system coupling polyoxometalates with deep eutectic solvents for selective aerobic oxidation desulfurization

Mingyue Chi,Zhiguo Zhu,Lulu Sun,Ting Su,Weiping Liao,Changliang Deng,Yuchao Zhao,Wanzhong Ren,Hongying Lü

Designing green and efficient catalytic system under extremely mild conditions with high atom economy is always desired in practical applications. In this study, an innovative and efficient biomimetic catalytic system coupling polyoxometalate (POM, Anderson-type Na 3 H 6 CrMo 6 O 24 ) with deep eutectic solvents (DESs) is proposed. This coupled system is applied for oxidation desulfurization, which exhibited extraordinary desulfurization performances at the extremely low temperature of 60 °C with the ambient pressure using oxygen as the oxidant. The desulfurization process follows the extraction-oxidation mechanism, during which POM severed as the electron transfer mediator is essential for highly efficient aerobic oxidation desulfurization. The deactivation of this catalytic system after reuse for four times was likely derived from the transformation of Na 3 H 6 CrMo 6 O 24 POM crystal structure. In addition, the incomparable desulfurization performances of this biomimetic system in commercially available diesel further strongly confirm the potential application on an industrial scale. More importantly, this work is helpful in the precisely design and development of biomimetic coupled systems for catalytic applications under extremely mild conditions.

CAS / MDL: 629-59-4
研究领域: 化学 · 环境科学 · 催化材料
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Biomimetic inspired porphyrin-based nanoframes for highly efficient photocatalytic CO2 reduction

Shujie Liang,Xiaohui Zhong,Zuqi Zhong,Bin Han,Weiyi Chen,Kainan Song,Hong Deng,Zhang Lin

The development of biomimetic catalysis for efficient photoreduction of CO 2 is an effective alternative to address energy problems. However, amelioration on the construction of biomimetic catalysts for elevated photocatalytic performance is still challenging and demanded. Herein, a bioinspired artificial photosynthesis system is constructed based on ZrO 2 nanoframes (ZFs) and metalloporphyrin to mimic the morphology of trees. The robust backbone of the framework and the bio-inspiring porphyrins anchored on the surface of ZFs function as the strong trunk and well-ordered leaves of a tree, respectively. The biomimetic system achieves an evolution yield of 35.3 μmol during 3 h reaction with 93.1% CO selectivity and 1.84% CO apparent quantum efficiency ( A.Q.E. ), which is about 60.8 times larger than that of pure porphyrin (Ni) (0.58 μmol). Detailed analysis reveals that the catalytic system could not only achieve fast separation of the photogenerated carriers and effective CO 2 activation but also possess suitable energy levels, which could efficiently transfer electrons to the Ni catalytic sites to improve the photocatalytic activity. Furthermore, the good recycling tests could be explained by the robust supporting of frameworks as well as the strong binding of the Zr atoms and carboxyl groups of porphyrins. This work presents a simple model of biomimetic catalysts and outlines possible strategies for other biomimetic manufactures.

CAS / MDL: 1291-32-3 14609-54-2
研究领域: 材料科学 · 环境科学 · 化学工程
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY · 2025 · IF 6

Construction of CeO2-MOF nanorods with oxygen vacancies for nanozyme catalytic antibacterial application

Meinan Yang,Nan Wang,Xu Wang,Ruiyong Zhang,Ini-lbehe Nabuk Etim,Mei-E. Yue,Jizhou Duan,Baorong Hou,Wolfgang Sand

Oxygen vacancies can provide active sites for catalysts, promoting catalytic activity. However, there are fewer nanozyme catalysts with oxygen vacancies. In this study, CeO 2 metal–organic framework (CeO 2 -MOF) nanorods with oxygen vacancies are synthesized through a simple hydrothermal and calcination processes. The obtained CeO 2 -MOFs exhibit excellent nanozyme catalytic activity for antibacterial applications. The CeO 2 -MOF nanorods demonstrate intrinsic haloperoxidase-like activity by catalyzing the bromination of organic signaling compounds, outperforming the catalytic properties of pure CeO 2 . The activity of CeO 2 -MOF (6) is the best because of its large specific surface area of 103.638 m 2 /g, surpassing that of CeO 2 at 74.752 m 2 /g. The oxygen vacancies are crucial in regulating the electronic structure of CeO 2 -MOFs, thereby improving the catalytic performance. The experiments of multiple substrates show that CeO 2 -MOF (6) exhibits good stability and recyclability. Additionally, CeO 2 -MOF (6) can catalyze the oxidation of Br - with H 2 O 2 to the corresponding hypobromous acid (HBrO), which exhibits strong antibacterial activity against typical marine bacteria ( Pseudomonas aeruginosa ). This study expands the range of biomimetic enzyme materials. It provides an efficient and green perspective and strategy for developing antibacterial and antifouling biomimetic catalysts, which offers a sustainable alternative for industrial applications in marine coatings and environmental protection.

CAS / MDL: 10294-41-4 143-74-8
研究领域: 材料科学 · 生物学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2017 · IF 6.216

A novel method for ultra-deep desulfurization of liquid fuels at room temperature

Hongya Liu,Shuxiang Bao,Zutong Cai,Tiefeng Xu,Nan Li,Lulin Wang,Haixiang Chen,Wangyang Lu,Wenxing Chen

A biomimetic catalytic system composed of iron hexadecachlorophthalocyanine (FePcCl 16 ), hydrogen peroxide (H 2 O 2 ), H 2 O and pyridine exhibited high activity for ultra-deep removal of dibenzothiophene (DBT) in model oil containing n-octane. The conversion of DBT was up to 100% after 60   min operation at room temperature. In addition, the FePcCl 16 catalyst could be recycled for more than 23 times without noticeable decrease on the conversion of DBT. Moreover, the activation energy evaluated through Arrhenius’ equation was found to be equal to 25.5   kJ/mol. Nitrogen-containing compounds such as pyridine, quinoline, and acridine, naturally existing in many kinds of fuel oil, had previously been considered to inhibit the oxidative desulfurization (ODS) process. Surprisingly, these organonitrogen compounds could actually accelerate the conversion rate of DBT in this catalytic system. Mechanistic studies revealed that the high-valent iron(IV)-oxo species were the main active intermediate via the heterolytic O–O bond cleavage of the putative iron(II)-hydroperoxo species. Pyridine binding to iron(II)-hydroperoxo complexes was demonstrated to facilitate the generation of high-valent iron(IV)-oxo species and enhance the reactivity of high-valent iron(IV)-oxo species in ODS.

研究领域: 化学工程 · 催化科学 · 环境科学
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CATALYSIS LETTERS · 2018 ·Vol. 148 ·期 9 ·2636-2642 · IF 2.911

Biomimetic Cleavage of Aryl–Nitrogen Bonds in N-Arylazoles Catalyzed by Metalloporphyrins

Yu Zongjiang,Zhai Guoqing,Xian Mo,Lu Ming,Wang Pengcheng,Jiang Tao,Xu Chao,Sun Weizhi

The cleavage of C–N single bonds of N -containing compounds provides either an excellent nitrogen source or an excellent carbon source. In this study, an efficient metalloporphyrins/H 2 O 2 cleavage of C–N bonds of arylpyrazoles was investigated. The effects of different factors, including different catalysts, catalyst dosages, H 2 O 2 dosages, reaction temperature and reaction time were studied. The experimental results showed that the optimal catalyst was FeTPPCl, and the yield of pyrazole derivatives could reach up to 12.3%, which was fourfold higher than hemin catalyzed reaction and closed to ceric ammonium nitrate catalyzed reaction, respectively. Compared with transition-metal-catalyzed and strong-oxidization cleavage of C–N bonds, this protocol is characterized by environmentally-friendly, stable, mild reaction conditions and simplified operation procedures. Graphical Abstract

CAS / MDL: 16009-13-5 9003-99-0
研究领域: 有机化学 · 催化化学
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