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A seawater throttle on H-2 production in Precambrian serpentinizing systems 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2020, 117 (26) : 14756-14763
作者:  Tutolo, Benjamin M.;  Seyfried, William E., Jr.;  Tosca, Nicholas J.
收藏  |  浏览/下载:9/0  |  提交时间:2020/06/22
serpentinization  Precambrian  atmosphere redox state  origins of life  
Nation-wide estimation of groundwater redox conditions and nitrate concentrations through machine learning 期刊论文
ENVIRONMENTAL RESEARCH LETTERS, 2020, 15 (6)
作者:  Knoll, Lukas;  Breuer, Lutz;  Bach, Martin
收藏  |  浏览/下载:11/0  |  提交时间:2020/07/02
groundwater quality  nitrate pollution  redox conditions  random forest  uncertainty  large-scale  
Recycling and metabolic flexibility dictate life in the lower oceanic crust 期刊论文
NATURE, 2020, 579 (7798) : 250-+
作者:  Zhou, Peng;  Yang, Xing-Lou;  Wang, Xian-Guang;  Hu, Ben;  Zhang, Lei;  Zhang, Wei;  Si, Hao-Rui;  Zhu, Yan;  Li, Bei;  Huang, Chao-Lin;  Chen, Hui-Dong;  Chen, Jing;  Luo, Yun;  Guo, Hua;  Jiang, Ren-Di;  Liu, Mei-Qin;  Chen, Ying;  Shen, Xu-Rui;  Wang, Xi;  Zheng, Xiao-Shuang;  Zhao, Kai;  Chen, Quan-Jiao;  Deng, Fei;  Liu, Lin-Lin;  Yan, Bing;  Zhan, Fa-Xian;  Wang, Yan-Yi;  Xiao, Geng-Fu;  Shi, Zheng-Li
收藏  |  浏览/下载:37/0  |  提交时间:2020/05/13

The lithified lower oceanic crust is one of Earth'  s last biological frontiers as it is difficult to access. It is challenging for microbiota that live in marine subsurface sediments or igneous basement to obtain sufficient carbon resources and energy to support growth(1-3) or to meet basal power requirements(4) during periods of resource scarcity. Here we show how limited and unpredictable sources of carbon and energy dictate survival strategies used by low-biomass microbial communities that live 10-750 m below the seafloor at Atlantis Bank, Indian Ocean, where Earth'  s lower crust is exposed at the seafloor. Assays of enzyme activities, lipid biomarkers, marker genes and microscopy indicate heterogeneously distributed and viable biomass with ultralow cell densities (fewer than 2,000 cells per cm(3)). Expression of genes involved in unexpected heterotrophic processes includes those with a role in the degradation of polyaromatic hydrocarbons, use of polyhydroxyalkanoates as carbon-storage molecules and recycling of amino acids to produce compounds that can participate in redox reactions and energy production. Our study provides insights into how microorganisms in the plutonic crust are able to survive within fractures or porous substrates by coupling sources of energy to organic and inorganic carbon resources that are probably delivered through the circulation of subseafloor fluids or seawater.


  
In situ NMR metrology reveals reaction mechanisms in redox flow batteries 期刊论文
NATURE, 2020, 579 (7798) : 224-+
作者:  Ma, Jianfei;  You, Xin;  Sun, Shan;  Wang, Xiaoxiao;  Qin, Song;  Sui, Sen-Fang
收藏  |  浏览/下载:13/0  |  提交时间:2020/07/03

Large-scale energy storage is becoming increasingly critical to balancing renewable energy production and consumption(1). Organic redox flow batteries, made from inexpensive and sustainable redox-active materials, are promising storage technologies that are cheaper and less environmentally hazardous than vanadium-based batteries, but they have shorter lifetimes and lower energy density(2,3). Thus, fundamental insight at the molecular level is required to improve performance(4,5). Here we report two in situ nuclear magnetic resonance (NMR) methods of studying redox flow batteries, which are applied to two redox-active electrolytes: 2,6-dihydroxyanthraquinone (DHAQ) and 4,4 '  -((9,10-anthraquinone-2,6-diyl)dioxy) dibutyrate (DBEAQ). In the first method, we monitor the changes in the H-1 NMR shift of the liquid electrolyte as it flows out of the electrochemical cell. In the second method, we observe the changes that occur simultaneously in the positive and negative electrodes in the full electrochemical cell. Using the bulk magnetization changes (observed via the H-1 NMR shift of the water resonance) and the line broadening of the H-1 shifts of the quinone resonances as a function of the state of charge, we measure the potential differences of the two single-electron couples, identify and quantify the rate of electron transfer between the reduced and oxidized species, and determine the extent of electron delocalization of the unpaired spins over the radical anions. These NMR techniques enable electrolyte decomposition and battery self-discharge to be explored in real time, and show that DHAQ is decomposed electrochemically via a reaction that can be minimized by limiting the voltage used on charging. We foresee applications of these NMR methods in understanding a wide range of redox processes in flow and other electrochemical systems.


  
Redox-switchable carboranes for uranium capture and release 期刊论文
NATURE, 2020, 577 (7792) : 652-+
作者:  Marques, Joao C.;  Li, Meng;  Schaak, Diane;  Robson, Drew N.;  Li, Jennifer M.
收藏  |  浏览/下载:31/0  |  提交时间:2020/07/03

The uranyl ion (UO22+  U(vi) oxidation state) is the most common form of uranium found in terrestrial and aquatic environments and is a central component in nuclear fuel processing and waste remediation efforts. Uranyl capture from either seawater or nuclear waste has been well studied and typically relies on extremely strong chelating/binding affinities to UO22+ using chelating polymers(1,2), porous inorganic(3-5) or carbon-based(6,7) materials, as well as homogeneous(8) compounds. By contrast, the controlled release of uranyl after capture is less established and can be difficult, expensive or destructive to the initial material(2,9). Here we show how harnessing the redox-switchable chelating and donating properties of an ortho-substituted closo-carborane (1,2-(Ph2PO)(2)-1,2-C2B10H10) cluster molecule can lead to the controlled chemical or electrochemical capture and release of UO22+ in monophasic (organic) or biphasic (organic/aqueous) model solvent systems. This is achieved by taking advantage of the increase in the ligand bite angle when the closo-carborane is reduced to the nido-carborane, resulting in C-C bond rupture and cage opening. The use of electrochemical methods for uranyl capture and release may complement existing sorbent and processing systems.


Redox-switchable chelation is demonstrated for a carborane cluster molecule, leading to controlled chemical or electrochemical capture and release of uranyl in monophasic or biphasic model solvent systems.


  
Redox Chemistry and Molybdenum Burial in a Mesoproterozoic Lake 期刊论文
GEOPHYSICAL RESEARCH LETTERS, 2019, 46 (11) : 5871-5878
作者:  Rico, K. I.;  Sheldon, N. D.;  Gallagher, T. M.;  Chappaz, A.
收藏  |  浏览/下载:5/0  |  提交时间:2019/11/26
redox  molybdenum  Proterozoic  biogeochemistry  
Kinetic Control on the Depth Distribution of Superdeep Diamonds 期刊论文
GEOPHYSICAL RESEARCH LETTERS, 2019, 46 (4) : 1984-1992
作者:  Zhu, Feng;  Li, Jie;  Liu, Jiachao;  Lai, Xiaojing;  Chen, Bin;  Meng, Yue
收藏  |  浏览/下载:8/0  |  提交时间:2019/04/09
superdeep diamond  slab-mantle interaction  redox reaction  reaction kinetics  
Modeling Depth of the Redox Interface at High Resolution at National Scale Using Random Forest and Residual Gaussian Simulation 期刊论文
WATER RESOURCES RESEARCH, 2019, 55 (2) : 1451-1469
作者:  Koch, Julian;  Stisen, Simon;  Refsgaard, Jens C.;  Ernstsen, Vibeke;  Jakobsen, Peter R.;  Hojberg, Anker L.
收藏  |  浏览/下载:4/0  |  提交时间:2019/11/26
Water Resource Managment  Nitrate  Redox Conditions  Machine Learning  Random Forest  Geostatistics  
Photoelectric conversion on Earth's surface via widespread Fe- and Mn-mineral coatings 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2019, 116 (20) : 9741-9746
作者:  Lu, Anhuai;  Li, Yan;  Ding, Hongrui;  Xu, Xiaoming;  Li, Yanzhang;  Ren, Guiping;  Liang, Jing;  Liu, Yuwei;  Hong, Hao;  Chen, Ning;  Chu, Shengqi;  Liu, Feifei;  Wang, Haoran;  Ding, Cong;  Wang, Changqiu;  Lai, Yong;  Liu, Juan;  Dick, Jeffrey;  Liu, Kaihui;  Hochella, Michael F., Jr.
收藏  |  浏览/下载:14/0  |  提交时间:2019/11/27
phototrophic  mineral coatings  birnessite  solar energy  redox (bio)geochemistry  
Metallic iron limits silicate hydration in Earth’s transition zone 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2019, 116 (45) : 22526-22530
作者:  Feng Zhu;  Jie Li;  Jiachao Liu;  Junjie Dong;  and Zhenxian Liu
收藏  |  浏览/下载:9/0  |  提交时间:2019/11/27
mantle transition zone  water budget  redox reaction  mantle oxidation state  deep hydrogen cycle