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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2024 · IF 10.8

Ferroheme/Ferriheme Directly Involved in the Synthesis and Decomposition of Hydrazine as an Electron Carrier during Anammox

Zhenxin Wang,Qilin Yu,Zhiqiang Zhao,Yaobin Zhang

Anammox bacteria performed the reaction of NH4+ and NO with hydrazine synthase to produce N2H4, followed by the decomposition of N2H4 with hydrazine dehydrogenase to generate N2. Ferroheme/ferriheme, which serves as the active center of both hydrazine synthase and hydrazine dehydrogenase, is thought to play a crucial role in the synthesis and decomposition of N2H4 during Anammox due to its high redox activity. However, this has yet to be proven and the exact mechanisms by which ferroheme/ferriheme is involved in the Anammox process remain unclear. In this study, abiotic and biological assays confirmed that ferroheme participated in NH4+ and NO reactions to generate N2H4 and ferriheme, and the produced N2H4 reacted with ferriheme to generate N2 and ferroheme. In other words, the ferroheme/ferriheme cycle drove the continuous reaction between NH4+ and NO. Raman, ultraviolet–visible spectroscopy, and X-ray absorption fine structure spectroscopy confirmed that ferroheme/ferriheme is involved in the synthesis and decomposition of N2H4 via the core FeII/FeIII cycle. The mechanism of ferroheme/ferriheme participation in the synthesis and decomposition of N2H4 was proposed by density functional theory calculations. These findings revealed for the first time the heme electron transfer mechanisms, which are of great significance for deepening the understanding of Anammox.

研究领域: 微生物学 · 环境生物学 · 生物化学
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JOURNAL OF POWER SOURCES · 2014 · IF 5.211

Ni/La2O3 catalyst containing low content platinum–rhodium for the dehydrogenation of N2H4·H2O at room temperature

Song-Il O,Jun-Min Yan,Hong-Li Wang,Zhi-Li Wang,Qing Jiang

Ni/La 2 O 3 nanocatalyst with Pt and Rh content as low as 5 mol%, respectively, is successfully synthesized by a facile co-reduction method in the presence of hexadecyl trimethyl ammonium chloride aqueous solution under ambient atmosphere. Interestingly, the resulted Ni/La 2 O 3 catalyst with low cost exhibits excellent catalytic activity to dehydrogenation of hydrous hydrazine (N 2 H 4 ·H 2 O), producing hydrogen with 100% selectivity at room temperature (298 K), which represents a promising step toward the practical application for N 2 H 4 ·H 2 O system on fuel cells.

CAS / MDL: 112-02-7 20765-98-4
研究领域: 催化化学 · 能源材料科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2016 · IF 3.205

Rh–Ni nanoparticles immobilized on Ce(OH)CO3 nanorods as highly efficient catalysts for hydrogen generation from alkaline solution of hydrazine

Jianmin Chen,Qilu Yao,Jia Zhu,Xiangshu Chen,Zhang-Hui Lu

Bimetallic Rh–Ni nanoparticles (NPs) immobilized on the cerium hydroxide carbonate (Ce(OH)CO 3 ) have been successfully prepared by a facile co-reduction route, and characterized by XRD , SEM , TEM , EDX, ICP , XPS , and TG-DTA. The as-synthesized Rh–Ni/Ce(OH)CO 3 nanocomposites (NCs) with different metal compositions were applied as the highly efficient catalysts for hydrogen generation from the alkaline solution of hydrazine (N 2 H 4 ). Especially, the Rh 55 Ni 45 /Ce(OH)CO 3 NCs exerted the highly activity and 100% H 2 selectivity for the decomposition of hydrazine, providing high turnover frequency (TOF) values of 150 h −1  at 30 °C and 395 h −1  at 50 °C, respectively, relative high values for the metal catalysts . The activation energy for the decomposition of hydrazine catalyzed by Rh 55 Ni 45 /Ce(OH)CO 3 NCs was measured to be 38.8 kJ/mol, lower than most of the values reported for this reaction using many different catalysts. This excellent catalytic performance could be attributed to not only the strain and ligand effects between Rh and Ni, but also the strong interaction between RhNi NPs and Ce(OH)CO 3 support. Such a highly catalyst may greatly encourage the practical application of hydrazine as a hydrogen storage material.

CAS / MDL: 57-13-6 13569-65-8
研究领域: 材料科学 · 催化化学
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Defence Technology · 2025 · IF 5.9

Bimetallic MOF (Mn/Co) constructed by active dicyandiamide linker for a promising combustion catalyst of solid propellant

Mingcheng Ge,Xian Xu,Ze Su,Ye Zhong,Binfang Yuan,Huisheng Huang,Jianguo Zhang,Zhimin Li

Combustion catalyst is a key modifier for the performance of composite solid propellant. To exploit high-efficiency combustion catalyst, a fascinating bimetallic metal-organic framework [MnCo(EIM) 2 (DCA) 2 ] n (1) was constructed by an active dicyandiamide (DCA) linker, Mn 2+ , Co 2+ centers, and an 1-ethylimidazole (EIM) ligand. 1 possesses good thermal stability ( T p = 205 °C), high energy density ( E g = 24.34 kJ/g, E v = 35.93 kJ/cm 3 ), and insensitivity to impact and frictional stimulus. The catalytic effects of 1 contrasted to monometallic coordination compounds Mn(EIM) 4 (DCA) 2 (2) and Co(EIM) 4 (DCA) 2 (3) on the thermal decomposition of AP/RDX composite were investigated by a DSC method. The decomposition peak temperatures of AP and RDX of the composite decreased to 335.8 °Cand 206.4 °C, respectively, and the corresponding activation energy decreased by 27.3% and 43.6%, respectively, which are better than the performances of monometallic complexes 2 and 3. The gas products in the whole thermal decomposition stage of the sample were measured by TG-MS and TG-IR, and the catalytic mechanism of 1 to AP/RDX was further analyzed. This work reveal potential application of bimetallic MOFs in the composite solid propellants.

CAS / MDL: 10026-22-9 10377-66-9
研究领域: 材料科学 · 化学工程
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2021 ·Vol. 168 ·期 5 ·057526 · IF 4.316

Synthesis of Highly Dispersed CuPd@UiO-66-NH2 for Nonenzymatic Hydrazine Sensing

Mengmeng Xu,Yuhua Dong,Jianbin Zheng

In this article, a core–shell CuPd@UiO-66-NH2 composite material was synthesized by a double-solvent reduction method, and an N2H4 electrochemical sensor based on CuPd@UiO-66-NH2 was constructed. The relationship between the morphology, type, composition, size of the sensor interface composite material and its electrocatalytic performance and sensor response performance was studied, and a new method for detecting N2H4 was established. The surface properties and composition of the materials were studied by transmission electron microscope(TEM),energy dispersive X-ray spectroscopy(EDX) and X-ray diffraction spectroscopy(XRD). The results showed that the synthesized CuPd@UiO-66-NH2 has a regular 3D structure, particle dispersion, and uniform particle size, the particle size is about 90 nm. Electrochemical performance studies showed the sensor is made into detecting N2H4 in a linear range of 0.25 μM ∼ 1.39 mM, with a sensitivity of 386.7 μA·mM−1·cm−2, and a detection limit of 0.08 μM(S/N = 3). Compared with other electrochemical sensors based on metal nanoparticles to detect N2H4, the new sensor exhibited a wider linear range; and its sensitivity was 3 times of that obtained by the Cu-BTC/OMC/GCE. So, the sensor can be used as a potential sensing material to detect hydrazine.

研究领域: 材料科学 · 分析化学 · 电化学
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Food Analytical Methods · 2013 ·Vol. 7 ·期 2 ·308-317 · IF 1.969

Simultaneous Determination of Trimethoprim and Diaveridine in Tissues of Chicken, Porcine, and Fish by Hydrophilic Interaction Liquid Chromatography–Tandem Mass Spectrometry

Luo Haoshi,Zhang Lifang,Xue Feiqun,Li Ying,Wang Xiaoyang,Fei Chenzhong,Zhang Chong

A sensitive liquid chromatography–tandem mass spectrometry method for simultaneous determination of trimethoprim and diaveridine in edible tissue samples (chicken and porcine muscle; liver, kidney, and fat tissues as well as fish muscle) was developed and validated in this study. Trimethoprim, diaveridine, and the internal standard trimethoprim-D 3 were extracted from samples using acetonitrile. The Oasis MCX Solid-Phase Extraction Cartridge was selected for cleaning up the extracts. Chromatographic separation was performed on a hydrophilic interaction liquid chromatography column with gradient elution. The analytes were determined using triple–quadrupole mass spectrometry in positive electrospray ionization and multiple reaction monitoring mode. The relative recoveries from spiked samples ranged from 82.5 to 117.2 %, with the relative standard deviations generally being below 15.4 %. Limits of detection and quantification for analytes were within 0.3–1 and 1–2 μg kg −1 , respectively. The proposed method was successfully applied to detect trimethoprim and diaveridine in real samples.

CAS / MDL: 540-69-2
研究领域: 分析化学 · 食品科学 · 兽医学
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Journal of Materials Chemistry A · 2016 ·Vol. 4 ·期 15 ·5616-5622 · IF 8.262

NiPt–MnOx supported on N-doped porous carbon derived from metal–organic frameworks for highly efficient hydrogen generation from hydrazine

Bingquan Xia,Teng Liu,Wei Luo,Gongzhen Cheng

Safe and efficient storage of hydrogen is the key issue for the hydrogen economy. Hydrazine monohydrate is regarded as a potential hydrogen carrier. Herein, we report a facile synthesis of NiPt–MnOx supported on nitrogen-doped porous carbon (NPC) derived from annealing metal–organic frameworks (MOFs) at different temperatures in Ar. Interestingly, the obtained (Ni3Pt7)0.5–(MnOx)0.5/NPC-900 exhibits superior catalytic activity toward dehydrogenation of an alkaline solution of hydrazine, with initial turnover frequency values of 706 and 120 h−1 at 323 K and room temperature, respectively. This excellent catalytic performance may have resulted from the synergistic electronic effect of NiPt and MnOx, the small size and high dispersion of NiPt–MnOx nanocatalysts, NPC as an excellent support with large pore volume, high surface area, high nitrogen content, electrical conductance, and also the high density of the metal-N active sites between NiPt–MnOx and NPC.

CAS / MDL: 51-17-2
研究领域: 材料科学 · 催化化学
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Small Methods · 2020 ·Vol. 4 ·期 9 ·2000208 · IF 12.13

Rh2S3/N-Doped Carbon Hybrids as pH-Universal Bifunctional Electrocatalysts for Energy-Saving Hydrogen Evolution

Chaoxiong Zhang,Haoxuan Liu,Yifan Liu,Xijun Liu,Yuying Mi,Ruijie Guo,Jiaqiang Sun,Haihong Bao,Jia He,Yuan Qiu,Junqiang Ren,Xiangjun Yang,Jun Luo,Guangzhi Hu

Using hydrazine oxidation reaction (HzOR) to replace the oxygen evolution reaction is an effective way to decrease the overpotential of the anodic reaction in overall water splitting (OWS), facilitating cost-effective and safe hydrogen production. Herein, Rh 2 S 3 /N-doped carbon hybrids (Rh 2 S 3 /NC) are first reported as novel and efficient bifunctional electrocatalysts for hydrazine-assisted hydrogen generation over a wide pH range. Specifically, Rh 2 S 3 /NC exhibits low overpotentials for the hydrogen evolution reaction (HER) in alkaline (38 mV), neutral (46 mV), and acidic (21 mV) electrolytes, to reach the current density of 10 mA cm −2 , and maintains the activities over 70 h. Meanwhile, Rh 2 S 3 /NC also displays competitive HzOR performance at all-pH electrolytes. Thus, serving as a bifunctional electrocatalyst for both HER and HzOR, Rh 2 S 3 /NC shows overwhelming-Pt/C performance in three electrolytes, and can save over 93.3%, 85.2%, and 78.3% energy consumption compared to the corresponding OWS system. Moreover, theoretical calculations confirm that Rh 2 S 3 /NC owns low free-energy changes of the H adsorption and the dehydrogenation of adsorbed NHNH both of which are beneficial to enhance catalytic activity. This work develops a novel bifunctional electrocatalyst with free pH-dependent condition for the hydrazine-assisted electrolysis system to furtherly reduce the cost of massive industrial H 2 production.

CAS / MDL: 1310-58-3
研究领域: 材料科学 · 能源化学 · 催化科学
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JOURNAL OF CATALYSIS · 2021 · IF 7.92

An efficient chiral porous catalyst support – Hypercrosslinked amino acid polymer

Yaodong Wang,Lijia Liu,Kexiao Sang,Yudan Wang,Chunhong Zhang,Hongxing Dong,Jianwei Bai

The application of asymmetric catalysis in industrial processes is limited by the high cost of chiral ligands and the difficulty associated with recovering precious metal catalysts. Here, based on a FeCl 3 -catalyzed Friedel–Crafts alkylation reaction, an aromatic amino acid was crosslinked with 4,4′-bis(chloromethyl)-1,1′-biphenyl to produce a novel porous chiral catalyst support, hypercrosslinked amino acid polymer (HCP-AA). Subsequently, metal catalysts were loaded on HCP-AA through the coordination of the metal ion with amino acid residues to generate heterogeneous asymmetric catalysts, HCP-AA-M. The resulting catalysts were characterized by scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, and Fourier transform infrared spectroscopy. The HCP-AA-M samples were employed to catalyze the heterogeneous asymmetric reaction, and they achieved high enantioselectivities (up to 99% ee). Meanwhile, the catalysts could be readily recovered through filtration, and they exhibited good recycling performances. The results suggested that the utilization of inexpensive amino acids as raw materials for producing porous chiral supports for recyclable high-performance asymmetric catalysts is an effective strategy.

研究领域: 有机化学 · 材料科学 · 催化化学
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SENSORS AND ACTUATORS B-CHEMICAL · 2020 · IF 7.1

A novel dual-response chemosensor for bioimaging of Exogenous/Endogenous hypochlorite and hydrazine in living cells, Pseudomonas aeruginosa and zebrafish

Xiaojun He,Zaian Deng,Wei Xu,Yahui Li,Chuchu Xu,Hong Chen,Jianliang Shen

Hypochlorite (ClO − ) and hydrazine (N 2 H 4 ) were poisonous to the biological environment. Accurate and sensitive identification of ClO − and N 2 H 4 in biological and environmental systems was essential to reveal their various physiological and pathological functions. Herein, a dual-response chemosensor, HNTBA , was developed for quantitative monitoring and visualization of ClO − and N 2 H 4 in vitro and in vivo via fluorescence turn-on strategy. With the addition of ClO − /N 2 H 4 , fluorescence “OFF–ON” response was obtained for the sensor as a result of specific ClO − /N 2 H 4 -triggered C C bond cleavage reaction with converted to the corresponding aldehyde and hydrazone, which responding mechanism was verified by DFT calculation. Additionally, HNTBA features rapid response (<30 s) and low limit of detection (nanomole), high sensitivity and selectivity toward ClO − /N 2 H 4 over other analytes, which allow it to be used for quantification of ClO − /N 2 H 4 in a simulated physiological condition. Fluorescence imaging using HNTBA sensor was taken to monitor the exogenous/endogenous ClO − levels in hPDLCs and RAW 264.7 cells in a concentration-dependent manner. Notably, HNTBA exhibits high effectiveness for early assessment of the treatment response of ClO − -mediated in cells with N-acetylcysteine ( NAC ) and lipopolysaccharide (LPS). Moreover, HNTBA can be used to visualize N 2 H 4 in live cells from blue channels with good performance. The outstanding sensing performances of HNTBA sensor enabled fast tracking of ClO − and N 2 H 4 in Pseudomonas aeruginosa and zebrafish with fluorescence light up, and it could be further applied to a paper strip. The results demonstrate that HNTBA was a powerful tool to monitor ClO − and N 2 H 4 in biosystems and environmental.

研究领域: 生物化学 · 医学 · 环境科学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2019 · IF 4.784

Physicochemical characterization of Gracilaria chouae sulfated polysaccharides and their antioxidant potential

Bilal Muhammad Khan,Hua-Mai Qiu,Xue-Fei Wang,Zhuo-Yan Liu,Jia-Yan Zhang,Yan-Jun Guo,Wei-Zhou Chen,Yang Liu,Kit-Leong Cheong

A complete absence of the physicochemical characterization of Gracilaria chouae polysaccharides (GCP) and its corresponding bioactivities urged the need for this study. It was found that GCP is a heteropolysaccharide which exists in linear random coil conformation. It contained a sulfate content of 7.9% in addition to 52.63% total sugar content and 9.62% galacturonic acid. Galactose and 3,6-anhydrogalactose were found in a molar ratio of 1.0:0.6. Its setting and melting points were determined as 41.3 and 71.7 °C, respectively, which makes it a suitable candidate for industrial processing where further heating is required and/or where the end-product needs to have extended shelf life in hot climate. GCP demonstrated 2,2-diphenyl-1-picrylhydrazyl, 2,2′-azino-bis and hydroxyl radical scavenging activity (36.86, 27.42 and 19.07% at 3 mg·ml −1 ). Moreover, the results also suggested its potential use as a prebiotic due to its perceived high fermentability.

CAS / MDL: 75-05-8 76-05-1 69-72-7
研究领域: 海洋生物学 · 药学 · 食品科学 · 生物化学
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