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- Ardo, Shane, et al.
(författare)
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Pathways to electrochemical solar-hydrogen technologies
- 2018
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Ingår i: Energy & Environmental Science. - : Royal Society of Chemistry. - 1754-5692 .- 1754-5706. ; 11:10, s. 2768-2783
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Forskningsöversikt (refereegranskat)abstract
- Solar-powered electrochemical production of hydrogen through water electrolysis is an active and important research endeavor. However, technologies and roadmaps for implementation of this process do not exist. In this perspective paper, we describe potential pathways for solar-hydrogen technologies into the marketplace in the form of photoelectrochemical or photovoltaic-driven electrolysis devices and systems. We detail technical approaches for device and system architectures, economic drivers, societal perceptions, political impacts, technological challenges, and research opportunities. Implementation scenarios are broken down into short-term and long-term markets, and a specific technology roadmap is defined. In the short term, the only plausible economical option will be photovoltaic-driven electrolysis systems for niche applications. In the long term, electrochemical solar-hydrogen technologies could be deployed more broadly in energy markets but will require advances in the technology, significant cost reductions, and/ or policy changes. Ultimately, a transition to a society that significantly relies on solar-hydrogen technologies will benefit from continued creativity and influence from the scientific community.
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| 2. |
- Schroeter, M., et al.
(författare)
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Exciton-vibrational coupling in the dynamics and spectroscopy of Frenkel excitons in molecular aggregates
- 2015
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Ingår i: Physics Reports. - : Elsevier BV. - 0370-1573. ; 567, s. 1-78
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Forskningsöversikt (refereegranskat)abstract
- The influence of exciton-vibrational coupling on the optical and transport properties of molecular aggregates is an old problem that gained renewed interest in recent years. On the experimental side, various nonlinear spectroscopic techniques gave insight into the dynamics of systems as complex as photosynthetic antennae. Striking evidence was gathered that in these protein-pigment complexes quantum coherence is operative even at room temperature conditions. Investigations were triggered to understand the role of vibrational degrees of freedom, beyond that of a heat bath characterized by thermal fluctuations. This development was paralleled by theory, where efficient methods emerged, which could provide the proper frame to perform non-Markovian and non-perturbative simulations of exciton-vibrational dynamics and spectroscopy. This review summarizes the state of affairs of the theory of exciton-vibrational interaction in molecular aggregates and photosynthetic antenna complexes. The focus is put on the discussion of basic effects of exciton-vibrational interaction from the stationary and dynamics points of view. Here, the molecular dimer plays a prominent role as it permits a systematic investigation of absorption and emission spectra by numerical diagonalization of the exciton-vibrational Hamiltonian in a truncated Hilbert space. An extension to larger aggregates, having many coupled nuclear degrees of freedom, becomes possible with the Multi-Layer Multi-Configuration Time-Dependent Hartree (ML-MCTDH) method for wave packet propagation. In fact it will be shown that this method allows one to approach the limit of almost continuous spectral densities, which is usually the realm of density matrix theory. Real system-bath situations are introduced for two models, which differ in the way strongly coupled nuclear coordinates are treated, as a part of the relevant system or the bath. A rather detailed exposition of the Hierarchy Equations Of Motion (HEOM) method will be given in terms of a stochastic decoupling ansatz. This method has become the standard in exciton-vibrational theory and illustrative examples will be presented as well as a comparison with ML-MCTDH. Applications will be shown for generic model systems as well as for small aggregates mimicking those formed by perylene bisimide dyes. Further, photosynthetic antenna complexes will be discussed, including spectral densities and the role of exciton-vibrational coupling in two-dimensional electronic spectroscopy. (C) 2014 Elsevier B.V. All rights reserved.
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| 3. |
- Schulze, E D, et al.
(författare)
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The European carbon balance. Part 4: integration of carbon and other trace-gas fluxes
- 2010
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Ingår i: GLOBAL CHANGE BIOLOGY. - : Blackwell Publishing Ltd. - 1354-1013 .- 1365-2486. ; 16:5, s. 1451-1469
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Forskningsöversikt (refereegranskat)abstract
- Overviewing the European carbon (C), greenhouse gas (GHG), and non-GHG fluxes, gross primary productivity (GPP) is about 9.3 Pg yr-1, and fossil fuel imports are 1.6 Pg yr-1. GPP is about 1.25% of solar radiation, containing about 360 x 1018 J energy - five times the energy content of annual fossil fuel use. Net primary production (NPP) is 50%, terrestrial net biome productivity, NBP, 3%, and the net GHG balance, NGB, 0.3% of GPP. Human harvest uses 20% of NPP or 10% of GPP, or alternatively 1 parts per thousand of solar radiation after accounting for the inherent cost of agriculture and forestry, for production of pesticides and fertilizer, the return of organic fertilizer, and for the C equivalent cost of GHG emissions. C equivalents are defined on a global warming potential with a 100-year time horizon. The equivalent of about 2.4% of the mineral fertilizer input is emitted as N2O. Agricultural emissions to the atmosphere are about 40% of total methane, 60% of total NO-N, 70% of total N2O-N, and 95% of total NH3-N emissions of Europe. European soils are a net C sink (114 Tg yr-1), but considering the emissions of GHGs, soils are a source of about 26 Tg CO2 C-equivalent yr-1. Forest, grassland and sediment C sinks are offset by GHG emissions from croplands, peatlands and inland waters. Non-GHGs (NH3, NOx) interact significantly with the GHG and the C cycle through ammonium nitrate aerosols and dry deposition. Wet deposition of nitrogen (N) supports about 50% of forest timber growth. Land use change is regionally important. The absolute flux values total about 50 Tg C yr-1. Nevertheless, for the European trace-gas balance, land-use intensity is more important than land-use change. This study shows that emissions of GHGs and non-GHGs significantly distort the C cycle and eliminate apparent C sinks.
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