BIOTECHNOLOGY LETTERS
·
2020
·Vol. 42
·期 3
·445-451
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IF 1.977
Zhang Lei,Xu Danyu,Kong Deyong,Ji Min,Shan Lianbin,Zhao Yongjiao
Objectives To investigate the effect of zero-valent iron and copper (Fe/Cu) micro-electrolysis on dark fermentative hydrogen production from glucose by a mixed bacterial consortium and the possible mechanisms of increasing hydrogen yield. Results Compared to zero-valent iron and activated carbon (Fe/C) micro-electrolysis, Fe/Cu micro-electrolysis could increase hydrogen yield by 32.2%, hydrogen production potential by 27.1%, and the maximum hydrogen production rate by 62.0%. Meanwhile, the number of ferrous ions released into the liquid phase with Fe/Cu micro-electrolysis was about 27.0% greater than that released by Fe/C micro-electrolysis, because the dispersion of copper on the surface of iron could markedly improve electrochemical corrosion activity. Metabolic analysis revealed that Fe/C micro-electrolysis promoted acetate formation, which may have been responsible for the observed improvement in fermentative hydrogen production. Further investigation indicated that Fe/Cu micro-electrolysis increased the activity of hydrogenases and stimulated the expression of the [FeFe]-hydrogenase gene. Conclusion Fe/Cu micro-electrolysis is better than Fe/C micro-electrolysis or Fe corrosion alone for dark fermentative hydrogen production.
研究领域:
环境工程
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微生物学
·
生物技术
✓ 已验证
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2020
·
IF 5.715
Zhen-Ni Yang,Ya-Nan Hou,Bo Zhang,Hao-Yi Cheng,Yang-Chun Yong,Wen-Zong Liu,Jing-Long Han,Shuang-Jiang Liu,Ai-Jie Wang
Biologically synthesized palladium nanoparticles (bio-Pd) have attracted considerable interest as promising green catalysts for environmental remediation. However, the mechanisms by which microorganisms produce bio-Pd remain unclear. In the present study, we investigated the roles of Shewanella oneidensis MR-1 and its NADH dehydrogenases and hydrogenases (HydA and HyaB) in bio-Pd production using formate as the electron donor. The roles of NADH dehydrogenases and hydrogenases were studied by inhibiting NADH dehydrogenases and using hydrogenase mutants (Δ hydA , Δ hyaB , and Δ hydA Δ hyaB ), respectively. The results showed ~97% reduction of palladium by S. oneidensis MR-1 after 24 h using 250 μM palladium and 500 μM formate. Electron microscopy images showed the presence of bio-Pd on both the outer and cytoplasmic membranes of S. oneidensis MR-1. However, the inhibition of NADH dehydrogenases in S. oneidensis MR-1 resulted in only ~61% reduction of palladium after 24 h, and bio-Pd were not found on the outer membrane. The mutants lacking one or two hydrogenases removed 91–96% of palladium ions after 24 h and showed more cytoplasmic bio-Pd but less periplasmic bio-Pd. To the best of our knowledge, this is the first study to demonstrate the role of NADH dehydrogenases of S. oneidensis MR-1 in the formation of bio-Pd on the outer membrane. It also demonstrates that the hydrogenases (especially HyaB) of S. oneidensis MR-1 contribute to the formation of bio-Pd in the periplasmic space. This study provides mechanistic insights into the production of biogenic metal nanoparticles towards their possible use in industrial and environmental applications.
研究领域:
微生物学
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环境科学
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纳米生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2020
·
IF 6.146
Minglun Cheng,Xiongfei Zhang,Yong Zhu,Mei Wang
Photocatalytic reduction of CO 2 to CO is a promising approach for storing solar energy in chemicals and mitigating the greenhouse effect of CO 2 . Our recent studies revealed that [( μ -bdt)Fe 2 (CO) 6 ] ( 1 , bdt = benzene-1,2-dithiolato), a [FeFe]-hydrogenase model with a rigid and conjugate S-to-S bridge, was catalytically active for the selective photochemical reduction of CO 2 to CO, while its analogous complex [( μ -edt)Fe 2 (CO) 6 ] (2, edt = ethane-1,2-dithiolato) was inactive. In this study, it was found that the turnover number of 1 for CO evolution reached 710 for the 1 /[Ru(bpy) 3 ] 2+ /BIH (BIH = 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[ d ]-imidazole) system under optimal conditions over 4.5 h of visible-light irradiation, with a turnover frequency of 7.12 min −1 in the first hour, a high selectivity of 97% for CO, and an internal quantum yield of 2.8%. Interestingly, the catalytic selectivity of 1 can be adjusted and even completely switched in a facile manner between the photochemical reductions of CO 2 to CO and of protons to H 2 simply by adding different amounts of triethanolamine to the catalytic system. The electron transfer in the photocatalytic system was studied by steady-state fluorescence and transient absorption spectroscopy, and a plausible mechanism for the photocatalytic reaction was proposed.
研究领域:
化学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2015
·
IF 3.313
Diyang Zhu,Zhiyin Xiao,Xiaoming Liu
A number of fibrous membranes with cellulose acetate as a matrix and functionalised with diiron mimics of the diiron subunit of [FeFe]-hydrogenase were prepared by electrospinning technique . Four mimics, [Fe 2 (μ-edt) (CO) 6 ] ( 1 ), [Fe 2 {μ-SCH 2 CH(CH 2 OH)S}(CO) 6 ] ( 2 ), [Fe 2 {(μ-S) 2 (C 6 O 2 H 4 )}(CO) 6 ] ( 3 ) and [Fe 2 {μ-SCH 2 CH(OH)CH 2 (OH)} 2 (CO) 6 ] ( 4 ), bearing 0, 1, 2 and 4 hydroxyl group(s) were incorporated into the electrospun fibrous membranes ( EFM s). To improve the conductivity of the EFM s, graphene oxide was chemically gratified onto cellulose acetate. The resultant EFM s membranes were characterized using infrared spectroscopic, thermogravimetric and scanning electron microscopic techniques. The electrochemical behaviours and electrocatalytic performance on proton reduction of the membrane electrodes assembled from the EFM s showed in aqueous media that the membrane ( M2 ) containing complex 2 is most durable and exhibited the best catalytic performance. To the electrospinning system containing complex 2 was further doped with basic polymer PEI to enhance tentatively proton transfer during the electrocatalysis of proton reduction. Our results showed that the presence of PEI in the EFM s did improve the electrocatalytic performance of proton reduction, presumably due to the enhancement in proton transfer in the catalysis.
研究领域:
生物化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHEMISTRY COMMUNICATIONS
·
2009
·
IF 4.194
Xianghua Zeng,Zhimei Li,Zhiyin Xiao,Yanwei Wang,Xiaoming Liu
The synthesis and characterisation of two diiron hexacarbonyl complexes [Fe 2 (SXS)(CO) 6 ], 1 (SXS = (( − SCH 2 ) 2 C(CH 3 )CH 2 OCOFc, Fc = ferrocenyl group) and 2 (SXS = ( − SCH 2 CH 2 NHCOFc) 2 ), were described. By using intramolecularly integrated ferrocenyl group(s) in the complexes as an internal standard, the nature of two stepwise one-electron processes of the complexes coupled with a chemical reaction was clearly demonstrated. Examining how the reduction transformed into sole one-electron process with both increasing scanning rate under Ar/CO atmosphere and lowering temperature indicated conclusively that the reduction of both complexes couples to a chemical reaction which involves CO-loss.
研究领域:
无机化学
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生物无机化学
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2013
·Vol. 37
·期 5
·1437-1444
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IF 2.966
Shang Gao,Hongling Guo,Xiaojun Peng,Xing Zhao,Qian Duan,Qingcheng Liang,Dayong Jiang
A tris(morpholino)phosphine (TMP) ligand was introduced into the diiron dithiolate complexes in order to improve the hydro- and protophilicity of the iron-only hydrogenase active site models. Mono- and di-TMP substituted diiron complexes, (μ-pdt)[Fe(CO)3][Fe(CO)2(TMP)] (2, pdt = 1,3-propanedithiolato) and (μ-pdt) [Fe(CO)2(TMP)]2 (3), were synthesized and spectroscopically characterized. The coordination configuration of 3 was determined by single X-ray analysis. Temperature-dependent 1H and 31P NMR spectroscopy studies provided insight into the interconversion of the irondithiacyclohexane ring and the rotation of the [Fe(CO)2PR3] moieties for 2 and 3 in solution. The electrochemical properties of 2 and 3 were investigated in pure CH3CN and CH3CN–H2O mixtures in the absence and presence of acetic acid. Hydrogen production and the dependence of current on acid concentration indicated that complexes 2 and 3 exhibited electrocatalytic activities for proton reduction in both pure and H2O-containing CH3CN solutions. The current sensitivities, i.e., electrocatalytic activities, were demonstrated to be greater in CH3CN–H2O mixtures than in pure CH3CN. The most effective electrocatalytic activities of 2 and 3 were observed with 10% added water.
研究领域:
无机化学
·
催化化学
✓ 已验证
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2023
·
IF 9.8
Xing Yan,Jie Bu,Xiong Chen,Ming-Jun Zhu
Microbial extracellular respiration is an important energy metabolism on earth, which is significant for the elemental biogeochemical cycle. Herein, extracellular Fe(III) and electrode respiration were confirmed in Thermoanaerobacterium thermosaccharolyticum MJ2 . The intra/extracellular electron transfer (IET/EET) mechanism of MJ2 was investigated by comparative genomic analysis for the first time. Morphological characterization and electrochemical properties of anode illustrated that MJ2 generated bio-electricity by forming a biofilm. The respiration chain inhibition and enzyme activity tests showed that hydrogenase with cytochrome c (Cyt- c ) was involved in IET of MJ2 . Noteworthily, the exogenous Cyt- c increased hydrogenase activity to promote bio-electricity generation by 92.84 %. The Cyt- c gene synteny between MJ2 and another well-known exoelectrogen ( Thermincola potens JR ) indicated that Cyt- c bound to the outer membrane mediated the formation of biofilm involved in EET of MJ2 . This study broadened the understanding of microbial extracellular respiration diversity and provided new insights to explore the electron transfer pathways of exoelectrogens.
研究领域:
微生物学
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基因组学
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电化学
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生物地球化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Sulfur Chemistry
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2020
·
IF 1.963
Lin Yan,Jun Yang,Xu-Feng Liu,Yu-Long Li,Xing-Hai Liu,Zhong-Qing Jiang
In this article, two new binuclear iron compounds [Fe2(CO)5PPh(C6H11)2{µ-SCH2CH(CH2CH3)S}] (2) and [Fe2(CO)5PPh2(C6H11){µ-SCH2CH(CH2CH3)S}] (3), which can be regarded as the biomimics for the active site of [FeFe]-H2ases, have been synthesized by CO exchange of compound [Fe2(CO)6{μ-SCH2CH(CH2CH3)S}] (1) with cyclohexyldiph-enylphosphine or dicyclohexylphenylphosphine and their structures have been confirmed by spectroscopy, elemental analysis, and X-ray crystallography. They also exhibited good electrocatalytic activities for the generation of H2.
研究领域:
无机化学
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材料科学
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生物无机化学
✓ 已验证
DOI
高影响因子
ACS ES&T Engineering
·
2025
·
IF 6.7
Jin-Feng Ma,Feng-Ai Yang,Haonan Guo,Ya-Nan Hou,Zhihua Liu,Nanqi Ren,Ai-Jie Wang,Cong Huang
Biogenic PdAu nanoparticles (bio-PdAu NPs) synthesized by microorganisms exhibit remarkable catalytic activity relevant to environmental remediation. This study investigates the biosynthetic pathway of bio-PdAu NPs synthesized by Shewanella oneidensis MR-1, revealing that the bioreduction of Pd(II) and Au(III) follows first-order kinetics. Inhibition of NADH dehydrogenase (rotenone, Rot-PdAu), c-Cyts (diuron, Diu-PdAu), and hydrogenase (Cu2+, Cu-PdAu) decreased total metal-ion reduction efficiencies and Pd/Au composition, in which hydrogenases contributed most, followed by NADH dehydrogenase and c-Cyts. Notably, the presence of inhibitors affected the Au(III) reduction efficiency, altering particle size and composition. Statistical analysis indicated average particle sizes of 45.45, 50.15, and 13.16 nm for Rot-PdAu, Diu-PdAu, and Cu-PdAu, respectively, with a positive correlation to kinetic constants (R2 = 0.82). During biosynthesis, intracellular and extracellular pathways contributed 76.55 and 23.44%, respectively. For electrocatalytic hydrogen evolution reaction, the maximum current density (jmax) of bio-PdAu NPs exhibits substantially superior electrocatalytic performance compared to monometallic counterparts, with current densities approximately 1.8–3.2 times higher than individual bio-Pd or bio-Au systems. These findings deepen the understanding of the controlled synthesis pathways of bio-PdAu NPs and offer insights for developing biobimetallic NPs for environmental applications.
研究领域:
微生物学
·
纳米生物技术
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环境修复
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生物无机化学
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电催化
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Jinghao Wang,Wenmin Lin,Yuancai Chen,Yongyou Hu,Qijin Luo
Due to the excellent hydrogen affinity and high conductivity, palladium nanoparticles (Pd NPs) were considered as a potential strategy to regulate bacterial electron transfer and energy metabolism. Herein, Citrobacter freundii JH, capable of in-situ biosynthesizing Pd(0) NPs, was employed to promote Pt(IV) reduction. The results showed that the Pt(IV) reduction to Pt(II) was accomplished mainly via the flavins-mediated extracellular electron transfer (EET) process, while Pt(II) reduction to Pt(0) was limit step, and proceeded via two intracellular respiratory chains, including FDH/Hases-based short chain (S-chain) and typical CoQ-involved long respiratory chain ( L -chain). Noteworthily, the incorporation of Pd(0) NPs mainly diverted the electrons to S-chain (as high as 71.7%−73.4%) by improving the hydrogenases (Hases) activity. Furthermore, Pd(0) NPs could stimulate the secreting of flavins and the combination between flavins and cytochrome c (c-Cyt), which converted electron transfer manner of L -chain. Additionally, Pd(0) NPs might also act as alternative proton channels to improve the energy metabolism. These findings provided significant insights into the promotion by Pd(0) NPs in terms of electron generation, electron consumption and proton translocation.
研究领域:
纳米技术
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微生物学
·
生物化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2013
·Vol. 3
·期 44
·21848-21855
·
IF 2.562
Wan-Qian Guo,Shan-Shan Yang,Ji-Wei Pang,Jie Ding,Xian-Jiao Zhou,Xiao-Chi Feng,He-Shan Zheng,Nan-Qi Ren
In order to increase hydrogen yield and shorten the lag time, low frequency ultrasonic (LFU) pretreatment was applied to stimulate the bio-activity of the seed bacteria, using waste activated sludge as the inoculum. A pretreated, sterilized sludge sample was seeded as the substrate for bio-hydrogen production. A Unisense microsensor multimeter with a hydrogen microelectrode was employed to examine the hydrogenase activities at different ultrasonic densities and exposure times. The optimum conditions were achieved at an ultrasonic density of 125 W L−1 and a reaction time of 10 s. A maximum hydrogen yield of 13.03 mL H2/g TS was obtained by LFU pretreatment under these optimal conditions, which was 18% higher than that obtained when seeding the raw sludge sample. To gain a better understanding of the end product distribution, three-dimensional excitation–emission matrix (3D-EEM) fluorescence spectroscopy was performed to characterize the dissolved organic matter (DOM) and extracellular polymeric substances (EPS) in the sludge samples during the anaerobic fermentation process. Hydrogen production from NADH/NAD+ conversion was also proved by EEM.
研究领域:
环境工程
·
生物技术
·
微生物学
✓ 已验证
DOI
高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Yuanming Wang,Zepeng Kang,Lingling Zhang,Zhiguang Zhu
Understanding the interactions and immobilization of hydrogenase on electrodes is important for promoting interfacial electron transfer and developing high-performance H2/O2 biofuel cells. The soluble hydrogenase I from the hyperthermophilic archaeon Pyrococcus furiosus (PfSHI) is a promising [NiFe]-hydrogenase. However, the [NiFe]-hydrogenase–electrode interface has not been explored on a microcosmic scale due to its structural complexity. In this work, an in-depth study of the interplay between PfSHI and carbon nanotubes was conducted via electrochemical techniques combined with a quartz crystal microbalance and modeling analysis. Through the interfacial analysis, it was found that PfSHI adopted different conformations on differently charged electrodes, demonstrating that electrostatic interaction may play the predominant role. Further, direct bioelectrocatalysis of H2 oxidation was investigated on different hydrophilic/hydrophobic electrode surfaces, and the results suggested that a hydrophobic interaction was another key factor determining the orientation distribution of PfSHI on the electrode. Reorientation occurred when PfSHI was close to the hydrophobic surface, leading to a proper spatial conformation on the electrode. Finally, a biofuel cell with immobilized PfSHI in a favorable orientation was constructed, exhibiting a superior power output at 60 °C 2-fold higher than that in a previous study. This study elucidates the absorption mechanism of PfSHI on functionalized electrodes, highlights the electrochemical methodology for analyzing the fundamentals of complex interfacial environments, and sheds light on the construction of high-performance bioelectrocatalytic interfaces.
研究领域:
生物化学
·
电化学
·
纳米技术
·
生物物理学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）