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Persistence of soil organic carbon caused by functional complexity 期刊论文
NATURE GEOSCIENCE, 2020
作者:  Lehmann, Johannes;  Hansel, Colleen M.;  Kaiser, Christina;  Kleber, Markus;  Maher, Kate;  Manzoni, Stefano;  Nunan, Naoise;  Reichstein, Markus;  Schimel, Joshua P.;  Torn, Margaret S.;  Wieder, William R.;  Koegel-Knabner, Ingrid
收藏  |  浏览/下载:12/0  |  提交时间:2020/08/09
Mud in rivers transported as flocculated and suspended bed material 期刊论文
NATURE GEOSCIENCE, 2020
作者:  Lamb, Michael P.;  de Leeuw, Jan;  Fischer, Woodward W.;  Moodie, Andrew J.;  Venditti, Jeremy G.;  Nittrouer, Jeffrey A.;  Haught, Daniel;  Parker, Gary
收藏  |  浏览/下载:11/0  |  提交时间:2020/07/09
The age distribution of global soil carbon inferred from radiocarbon measurements 期刊论文
NATURE GEOSCIENCE, 2020
作者:  Shi, Zheng;  Allison, Steven D.;  He, Yujie;  Levine, Paul A.;  Hoyt, Alison M.;  Beem-Miller, Jeffrey;  Zhu, Qing;  Wieder, William R.;  Trumbore, Susan;  Randerson, James T.
收藏  |  浏览/下载:18/0  |  提交时间:2020/07/06
Tropical forest loss enhanced by large-scale land acquisitions 期刊论文
NATURE GEOSCIENCE, 2020, 13 (7) : 482-+
作者:  Davis, Kyle Frankel;  39;Angelo, Jampel;  39;Odorico, Paolo
收藏  |  浏览/下载:15/0  |  提交时间:2020/06/29
Millennial-scale hydroclimate control of tropical soil carbon storage 期刊论文
NATURE, 2020, 581 (7806) : 63-+
作者:  Lam, Tommy Tsan-Yuk;  Jia, Na;  Zhang, Ya-Wei;  Shum, Marcus Ho-Hin;  Jiang, Jia-Fu;  Zhu, Hua-Chen;  Tong, Yi-Gang;  Shi, Yong-Xia;  Ni, Xue-Bing;  Liao, Yun-Shi;  Li, Wen-Juan;  Jiang, Bao-Gui;  Wei, Wei;  Yuan, Ting-Ting;  Zheng, Kui;  Cui, Xiao-Ming;  Li, Jie;  Pei, Guang-Qian
收藏  |  浏览/下载:25/0  |  提交时间:2020/05/13

Over the past 18,000 years, the residence time and amount of soil carbon stored in the Ganges-Brahmaputra basin have been controlled by the intensity of Indian Summer Monsoon rainfall, with greater carbon destabilization during wetter, warmer conditions.


The storage of organic carbon in the terrestrial biosphere directly affects atmospheric concentrations of carbon dioxide over a wide range of timescales. Within the terrestrial biosphere, the magnitude of carbon storage can vary in response to environmental perturbations such as changing temperature or hydroclimate(1), potentially generating feedback on the atmospheric inventory of carbon dioxide. Although temperature controls the storage of soil organic carbon at mid and high latitudes(2,3), hydroclimate may be the dominant driver of soil carbon persistence in the tropics(4,5)  however, the sensitivity of tropical soil carbon turnover to large-scale hydroclimate variability remains poorly understood. Here we show that changes in Indian Summer Monsoon rainfall have controlled the residence time of soil carbon in the Ganges-Brahmaputra basin over the past 18,000 years. Comparison of radiocarbon ages of bulk organic carbon and terrestrial higher-plant biomarkers with co-located palaeohydrological records(6) reveals a negative relationship between monsoon rainfall and soil organic carbon stocks on a millennial timescale. Across the deglaciation period, a depletion of basin-wide soil carbon stocks was triggered by increasing rainfall and associated enhanced soil respiration rates. Our results suggest that future hydroclimate changes in tropical regions are likely to accelerate soil carbon destabilization, further increasing atmospheric carbon dioxide concentrations.


  
Molecular tuning of CO2-to-ethylene conversion 期刊论文
NATURE, 2020, 577 (7791) : 509-+
作者:  Li, Fengwang;  39;Brien, Colin P.
收藏  |  浏览/下载:11/0  |  提交时间:2020/07/03

The electrocatalytic reduction of carbon dioxide, powered by renewable electricity, to produce valuable fuels and feedstocks provides a sustainable and carbon-neutral approach to the storage of energy produced by intermittent renewable sources(1). However, the highly selective generation of economically desirable products such as ethylene from the carbon dioxide reduction reaction (CO2RR) remains a challenge(2). Tuning the stabilities of intermediates to favour a desired reaction pathway can improve selectivity(3-5), and this has recently been explored for the reaction on copper by controlling morphology(6), grain boundaries(7), facets(8), oxidation state(9) and dopants(10). Unfortunately, the Faradaic efficiency for ethylene is still low in neutral media (60 per cent at a partial current density of 7 milliamperes per square centimetre in the best catalyst reported so far(9)), resulting in a low energy efficiency. Here we present a molecular tuning strategy-the functionalization of the surface of electrocatalysts with organic molecules-that stabilizes intermediates for more selective CO2RR to ethylene. Using electrochemical, operando/in situ spectroscopic and computational studies, we investigate the influence of a library of molecules, derived by electro-dimerization of arylpyridiniums(11), adsorbed on copper. We find that the adhered molecules improve the stabilization of an '  atop-bound'  CO intermediate (that is, an intermediate bound to a single copper atom), thereby favouring further reduction to ethylene. As a result of this strategy, we report the CO2RR to ethylene with a Faradaic efficiency of 72 per cent at a partial current density of 230 milliamperes per square centimetre in a liquid-electrolyte flow cell in a neutral medium. We report stable ethylene electrosynthesis for 190 hours in a system based on a membrane-electrode assembly that provides a full-cell energy efficiency of 20 per cent. We anticipate that this may be generalized to enable molecular strategies to complement heterogeneous catalysts by stabilizing intermediates through local molecular tuning.


Electrocatalytic reduction of CO2 over copper can be made highly selective by '  tuning'  the copper surface with adsorbed organic molecules to stabilize intermediates for carbon-based fuels such as ethylene


  
Accelerated discovery of CO2 electrocatalysts using active machine learning 期刊论文
NATURE, 2020, 581 (7807) : 178-+
作者:  Lan, Jun;  Ge, Jiwan;  Yu, Jinfang;  Shan, Sisi;  Zhou, Huan;  Fan, Shilong;  Zhang, Qi;  Shi, Xuanling;  Wang, Qisheng;  Zhang, Linqi;  Wang, Xinquan
收藏  |  浏览/下载:88/0  |  提交时间:2020/07/03

The rapid increase in global energy demand and the need to replace carbon dioxide (CO2)-emitting fossil fuels with renewable sources have driven interest in chemical storage of intermittent solar and wind energy(1,2). Particularly attractive is the electrochemical reduction of CO2 to chemical feedstocks, which uses both CO2 and renewable energy(3-8). Copper has been the predominant electrocatalyst for this reaction when aiming for more valuable multi-carbon products(9-16), and process improvements have been particularly notable when targeting ethylene. However, the energy efficiency and productivity (current density) achieved so far still fall below the values required to produce ethylene at cost-competitive prices. Here we describe Cu-Al electrocatalysts, identified using density functional theory calculations in combination with active machine learning, that efficiently reduce CO2 to ethylene with the highest Faradaic efficiency reported so far. This Faradaic efficiency of over 80 per cent (compared to about 66 per cent for pure Cu) is achieved at a current density of 400 milliamperes per square centimetre (at 1.5 volts versus a reversible hydrogen electrode) and a cathodic-side (half-cell) ethylene power conversion efficiency of 55 +/- 2 per cent at 150 milliamperes per square centimetre. We perform computational studies that suggest that the Cu-Al alloys provide multiple sites and surface orientations with near-optimal CO binding for both efficient and selective CO2 reduction(17). Furthermore, in situ X-ray absorption measurements reveal that Cu and Al enable a favourable Cu coordination environment that enhances C-C dimerization. These findings illustrate the value of computation and machine learning in guiding the experimental exploration of multi-metallic systems that go beyond the limitations of conventional single-metal electrocatalysts.


  
Ice-nucleating ability of particulate emissions from solid-biomass-fired cookstoves: an experimental study 期刊论文
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2020, 20 (8) : 4951-4968
作者:  Korhonen, Kimmo;  Kristensen, Thomas Bjerring;  Falk, John;  Lindgren, Robert;  Andersen, Christina;  Carvalho, Ricardo Luis;  Malmborg, Vilhelm;  Eriksson, Axel;  Boman, Christoffer;  Pagels, Joakim;  Svenningsson, Birgitta;  Komppula, Mika;  Lehtinen, Kari E. J.;  Virtanen, Annele
收藏  |  浏览/下载:7/0  |  提交时间:2020/07/02
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.


  
Isotopic evidence for quasi-equilibrium chemistry in thermally mature natural gases 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2020, 117 (8) : 3989-3995
作者:  Thiagarajan, Nivedita;  Xie, Hao;  Ponton, Camilo;  Kitchen, Nami;  Peterson, Brian;  Lawson, Michael;  Formolo, Michael;  Xiao, Yitian;  Eiler, John
收藏  |  浏览/下载:7/0  |  提交时间:2020/05/13
stable isotopes  compound-specific isotope analysis  clumped isotopes  natural gas  methane