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The improvement and comparison of diffuse radiation models in different climatic zones of China 期刊论文
Atmospheric Research, 2021
作者:  Tingting Zhu, Jun Li, Liang He, Dingrong Wu, ... Qiang Yu
收藏  |  浏览/下载:11/0  |  提交时间:2021/02/17
Global distribution of sediment-hosted metals controlled by craton edge stability 期刊论文
NATURE GEOSCIENCE, 2020, 13 (7) : 504-+
作者:  Hoggard, Mark J.;  Czarnota, Karol;  Richards, Fred D.;  Huston, David L.;  Jaques, A. Lynton;  Ghelichkhan, Sia
收藏  |  浏览/下载:16/0  |  提交时间:2020/07/06
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


  
Extracellular electron transfer-dependent anaerobic oxidation of ammonium by anammox bacteria 期刊论文
NATURE COMMUNICATIONS, 2020, 11 (1)
作者:  Shaw, Dario R.;  Ali, Muhammad;  Katuri, Krishna P.;  Gralnick, Jeffrey A.;  Reimann, Joachim;  Mesman, Rob;  van Niftrik, Laura;  Jetten, Mike S. M.;  Saikaly, Pascal E.
收藏  |  浏览/下载:6/0  |  提交时间:2020/05/13
Measured greenhouse gas budgets challenge emission savings from palm-oil biodiesel 期刊论文
NATURE COMMUNICATIONS, 2020, 11 (1)
作者:  Meijide, Ana;  de la Rua, Cristina;  Guillaume, Thomas;  Roell, Alexander;  Hassler, Evelyn;  Stiegler, Christian;  Tjoa, Aiyen;  June, Tania;  Corre, Marife D.;  Veldkamp, Edzo;  Knohl, Alexander
收藏  |  浏览/下载:10/0  |  提交时间:2020/05/13
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:11/0  |  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.


  
Power generation from ambient humidity using protein nanowires 期刊论文
NATURE, 2020, 578 (7796) : 550-+
作者:  Luong, Duy X.;  Bets, Ksenia V.;  Algozeeb, Wala Ali;  Stanford, Michael G.;  Kittrell, Carter;  Chen, Weiyin;  Salvatierra, Rodrigo V.;  Ren, Muqing;  McHugh, Emily A.;  Advincula, Paul A.;  Wang, Zhe;  Bhatt, Mahesh;  Guo, Hua;  Mancevski, Vladimir;  Shahsavari, Rouzbeh;  Yakobson, Boris I.;  Tour, James M.
收藏  |  浏览/下载:85/0  |  提交时间:2020/07/03

Harvesting energy from the environment offers the promise of clean power for self-sustained systems(1,2). Known technologies-such as solar cells, thermoelectric devices and mechanical generators-have specific environmental requirements that restrict where they can be deployed and limit their potential for continuous energy production(3-5). The ubiquity of atmospheric moisture offers an alternative. However, existing moisture-based energy-harvesting technologies can produce only intermittent, brief (shorter than 50 seconds) bursts of power in the ambient environment, owing to the lack of a sustained conversion mechanism(6-12). Here we show that thin-film devices made from nanometre-scale protein wires harvested from the microbe Geobacter sulfurreducens can generate continuous electric power in the ambient environment. The devices produce a sustained voltage of around 0.5 volts across a 7-micrometre-thick film, with a current density of around 17 microamperes per square centimetre. We find the driving force behind this energy generation to be a self-maintained moisture gradient that forms within the film when the film is exposed to the humidity that is naturally present in air. Connecting several devices linearly scales up the voltage and current to power electronics. Our results demonstrate the feasibility of a continuous energy-harvesting strategy that is less restricted by location or environmental conditions than other sustainable approaches.


A new type of energy-harvesting device, based on protein nanowires from the microbe Geobacter sulforreducens, can generate a sustained power output by producing a moisture gradient across the nanowire film using natural humidity.


  
Satellite data reveal a common combustion emission pathway for major cities in China 期刊论文
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2019, 19 (7) : 4269-4288
作者:  Tang, Wenfu;  Arellano, Avelino F.;  Gaubert, Benjamin;  Miyazaki, Kazuyuki;  Worden, Helen M.
收藏  |  浏览/下载:7/0  |  提交时间:2019/11/26
Anthropogenic and natural drivers of a strong winter urban heat island in a typical Arctic city 期刊论文
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2018, 18 (23) : 17573-17587
作者:  Varentsov, Mikhail;  Konstantinov, Pavel;  Baklanov, Alexander;  Esau, Igor;  Miles, Victoria;  Davy, Richard
收藏  |  浏览/下载:4/0  |  提交时间:2019/04/09
Light-driven fine chemical production in yeast biohybrids 期刊论文
SCIENCE, 2018, 362 (6416) : 813-+
作者:  Guo, Junling;  Suastegui, Miguel;  Sakimoto, Kelsey K.;  Moody, Vanessa M.;  Xiao, Gao;  Nocera, Daniel G.;  Joshi, Neel S.
收藏  |  浏览/下载:3/0  |  提交时间:2019/11/27