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Solar Fuel Production for a Sustainable Energy Future: Highlights of a Symposium on Renewable Fuels from Sunlight and Electricity by Heli Wang, Deryn Chu, and Eric L

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Solar Fuel Production for a Sustainable Energy Future: Highlights of a Symposium on Renewable Fuels from Sunlight and Electricity by Heli Wang, Deryn Chu, and Eric L Solar Fuel Production for a Sustainable Energy Future: Highlights of a Symposium on Renewable Fuels from Sunlight and Electricity by Heli Wang, Deryn Chu, and Eric L. Miller ynthesis of fuels from sunlight, water 222nd ECS Meeting in Honolulu in October. In this paper, an emphasis is placed on and carbon dioxide, without competing Over 130 abstracts were received for this the summary of the presentations for solar Swith food production, is an important symposium. The symposium attendees came fuels production. We will highlight some of route for sustainable development beyond from North America, Europe, and Asia. The the presentations that reflected the research fossil fuels. The magnitude of the challenge research theme of this symposium focused progress in this field. is very significant that requires scientific on the development of materials and devices Metal oxides are the most studied breakthroughs in materials and processing for hydrogen generation and CO2 conversion semiconductor material group. While metal for creating economic opportunities.1 to fuels. One approach is to utilize the solar oxides are more stable in aqueous solutions, There are two straightforward conversion energy to produce fuels. Another approach key issues are wide band gap, band-edge pathways for conversion of solar energy is to utilize the electrical energy to generate mismatch and their intrinsic low STH to fuels.2 The most important one is the fuels with electrochemical devices. The efficiencies. A combinatorial screening might photoelectrochemical (PEC) hydrogen symposium presentations covered the be a relevant approach to search for metal production via water splitting, which following topics in both approaches: oxides with suitable band gap.4 Different combines the electrical generation and tandem cells5-9 have been developed to solve • solar energy materials; electrolysis into a single system. The other the band edge mismatch. In the keynote • photocatalysts; pathway is replicating plant photosynthesis speech, Akihiko Kudo at Tokyo University • photo electrochemical cells (PECs); process with water and CO . These direct of Science (Japan) highlighted the Z-scheme 2 • biological devices; solar fuel pathways, especially the PEC water type photocatalysts for water splitting with • solar concentrators; splitting approach, have attracted attention improved Rh-doped SrTiO and BiVO . One • solid oxide electrolysis cells (SOECs); 3 4 world-wide due to their renewable fuel the other hand, Lionel Vayssieres at Xi’an • solid oxide fuel cells (SOFCs); and generation and benefit to the environment. In Jiaotong University (China) introduced an • proton conductor electrolysis cells electrochemical and photoelectrochemical (PCECs) and fuel cells (PCFC). all-oxide quantum confinement approach to techniques, the electrodes combine with (continued on next page) catalysts, inhibitors, and an electrochemical flow reactor to convert CO2 to organic fuels. In PEC water splitting, the grand challenge of 10% solar-to-hydrogen (STH) efficiency and 10 year lifetime was defined A as the “holy grail of chemistry.”3 The requirements for a successful PEC water splitting device is displayed in Fig. 1, as shown with a p-type semiconductor case. To achieve efficient PEC water splitting at an illuminated semiconductor (SC), 1. the band gap (Eg) of the SC must be at least 1.6-1.7 eV since the theoretical H2O/H2 difference in equilibrium potentials be- tween water splitting reactions is 1.228 V at 25 °C. The overpotential must be sufficient for water splitting reactions, 1.23 eV but not over 2.2-2.3 eV in order to ab- hv 1.6-1.7 eV sorb the visible light; Counter 2. the band edges of the SC must straddle Electrode the water redox potentials; H2O/O2 3. the SC must meet the need of efficient charge generation/transfer in the bulk and fast reaction kinetics at the inter- face; and 4. the SC must be stable in aqueous solu- tions. It is challenging to develop materials that meet all the requirements of photoelectrodes/ p-type photocatalysts. To facilitate the research in photocatalysts and solar fuel production, Semiconductor a symposium on “Renewable Fuels from Sunlight and Electricity” was held at the FIG. 1. Schematic of the PEC water splitting process at illuminated p-type semiconductor. The Electrochemical Society Interface • Summer 2013 69 Wang, Chu, and Miller (continued from previous page) Naturally, there is no single material efforts are still needed to design and explore that could meet all the requirements of new photocatalysts and PEC materials to solve the issue. The low solar-to-hydrogen photoelectrodes/photocatalysts for water meet the “holy grail” challenge.3 efficiency is related to wide band gap, light splitting; and this has challenged the PEC In CO2 reduction, the thermodynamically absorption, charge mobility, recombination, communities for decades. Multi-junction uphill nature of this reaction, coupled with interfacial kinetics, etc. To overcome this cells, quantum dots, and plasmonic metals the large activation energy associated hurdle, different approaches have been brought new opportunities for research and with the multi-electron and multi-proton discussed at the symposium, including development of PECs and photocatalysts. reduction, makes the conversion of CO2 a band gap engineering, doping and co- For example, Nianqiang (Nick) Wu, West big challenge.13 Thomas F. Jaramillo from doping, nanostructuring, and catalyst, etc. Virginia University, talked about the Stanford University observed a total of 16 Moreover, Nam-Gyu Park at Sungkyunkwan development of plasmonic nanostructures different CO2 reduction products (C1-C3) University (Korea) presented new solar for enhancing the photocatalysis. Plasmonic from a polycrystalline copper electrode, five energy materials and nanostructures in his nanostructures convert the solar energy to of which were presented at the meeting. They keynote talk. the plasmonic energy stored in the oscillating have expanded their studies to numerous Semiconductor materials such as III-V electrons. Such energy can transfer from the metals such as Pt, Au, Ag, Ni, Zn, and Fe, as metal to the semiconductor via a plasmonic- well as non-metal surfaces. Andrew Bocarsly and I-III-VI2 compounds have suitable band gaps and high efficiencies. The band induced resonant energy transfer (PIRET) from Princeton University presented the edge mismatch was successfully solved by process,11 leading to generation of electron- pyridinium catalyzed electrochemical 10 a tandem cell design. However, the trade- hole pairs in the semiconductor. The PIRET reduction of CO2 to methanol at illuminated off is the photo-corrosion of III-V materials is an unprecedented mechanism of plasmon- p-GaP photocathodes; with Faradaic in PEC hydrogen generation. Silicon enhanced photocatalysis, which provides the efficiencies exceeding 95%. From this materials have oxidation issue in the dark, guidelines for development of plasmonic effort, they proposed that the reduction of thus eliminating continuous application. photosensitizes for solar energy harvesting CO2 is initiated by a mediated charge transfer Naturally the surface modification devices. process, in which the one electron reduction and protection of the high efficient Government support plays a key role of pyridinium leads to the formation of semiconductors have been discussed in to foster PEC R&D. In his keynote talk, a carbamate intermediate. Protonated the symposium. In the keynote speech, Eric Miller of the Fuel Cell Technologies imidazole was also found to be an active John A. Turner, the National Renewable Program at the Office of Energy Efficiency catalyst for the conversion of CO2 to CO and Energy Laboratory (U.S.), addressed the and Renewable Energy of DOE (U.S.) formate in an aqueous electrolyte at an iron competition of PEC hydrogen production shared the “big picture” of the roles of pyrite electrode. vs. photovoltaic (PV) electrolysis, and hydrogen and fuel cells in diverse energy Paul Kenis’ group from the University of delivered cost and economic considerations portfolios. He illustrated the promises and Illinois at Urbana-Champaign has developed in selecting PEC materials. challenges of different renewable solar an electrochemical flow reactor for CO2 Krishnan Rajeshwar, University of Texas hydrogen technologies, and addressed reduction, in which the anode and cathode at Arlington (U.S.), after a short review on the need for national and international are separated by a flowing liquid electrolyte PEC efforts over generations, focused on collaborations for leveraging research to (Fig. 2). Owing to the differences in binding the economic preparation of new families meet these challenges. He presented the energy of intermediates by different particle techno-economic analysis, indicating the size, the reaction rate for CO reduction of metal oxides for water splitting and CO2 2 reduction in his keynote speech. Moreover, critical need for materials systems with increases upon the catalyst particle size characterization and theoretical approaches conversion efficiency exceeding 10% STH decrease from 200 to 5 nm, but then opened new windows for understanding efficiency (in many cases, even exceeding decreases upon the particle size decreasing the challenge and discovering new PEC the 20% mark) to meet the DOE hydrogen further to 1 nm. A thin, uniformly distributed, materials. The combined synthesis- cost threshold.12 This pushes the bar even and agglomerate-free catalyst layer is a key characterization-theory
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