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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:13/0  |  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


  
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.


  
What Triggers Streamflow for Intermittent Rivers and Ephemeral Streams in Low-Gradient Catchments in Mediterranean Climates 期刊论文
WATER RESOURCES RESEARCH, 2019
作者:  Gutierrez-Jurado, Karina Y.;  Partington, Daniel;  Batelaan, Okke;  Cook, Peter;  Shanafield, Margaret
收藏  |  浏览/下载:8/0  |  提交时间:2020/02/16
Intermittent Rivers and Ephemeral Streams  Streamflow generation  Integrated surface-subsurface modeling  Hydrological processes  
The impact of policy actions and future energy prices on the cost-optimal development of the energy system in Norway and Sweden 期刊论文
ENERGY POLICY, 2017, 106
作者:  Seljom, Pernille;  Tomasgard, Asgeir
收藏  |  浏览/下载:1/0  |  提交时间:2019/04/09
TIMES  Stochastic programming  Hydropower  Energy system  Intermittent electricity generation  Renewable energy  Investment model  
A novel inclusion of intermittent generation resources in long term energy auctions 期刊论文
ENERGY POLICY, 2017, 100
作者:  Marambio, Rodrigo;  Rudnick, Hugh
收藏  |  浏览/下载:0/0  |  提交时间:2019/04/09
Renewable energy  Energy auctions  Risk management  Intermittent generation