Abstract
Converting solar energy into power and hydrogen provides a promising pathway to fulfilling instantaneous electricity demand (power generation) as well as continuous demand via storing energy in chemical bonds (hydrogen generation). Co-generation of power and hydrogen is of great interest due to its potential to overcome expensive electricity storage in conventional PV plus battery systems. Both solar thermochemistry processes and photo-electrochemical cells (PECs) are extensively explored technologies to produce solar hydrogen. The key challenges for solar thermochemistry processes are extremely high operating temperature (~ 1500 oC) and low demonstrated efficiency (< 1% for hydrogen generation). For PECs, the limited solar absorption together with sluggish electrochemical reactions, especially for OER, leads to limited theoretical solar fuel generation. Operating PECs at high temperature will lead to decreased photovoltage and interface stability. Inspired by the thermally regenerative batteries, we propose a photo-thermo-electrochemical (PTEC) device that uses the solid oxide-based moderate high temperature cell (~1000 ℃) as the photo-absorber for simultaneously converting concentrated solar radiation into heat and generating fuel or power electrochemically driven by the discharging power from the low temperature cell (~700 ℃). PTEC device enables full solar spectrum utilization, highly favorable thermodynamics and kinetics, and cost-effectiveness. A continuous PTEC device has two working modes, which are voltage differential (VD) mode and current differential (CD) mode. The current-voltage characteristics of a PTEC device are shown in Figure 1. It mainly consists of five parts. A high temperature cell (HTC) serves as a solar absorber and a low temperature cell (LTC) serves as heat recovery. Besides, the opposite electrochemical reactions take place in two cells meaning that HTC and LTC can also function as a hydrogen production as well as an electricity generator component, respectively. Heat exchanger(s) is placed between the HTC and LTC and hot fluids pass through a heat exchanger before entering LTC to reduce heat losses to environment as well as reducing input solar energy. The VD mode and CD mode can be realized in PTECs via controlling of DC-DC converter. In order to identify the main parameters, we develop a multi-physics model based on finite element method, including mass, heat and charge transfer, and electrochemical reactions. In addition, heat exchange is modeled by solving energy balance equation, DC-DC convertor is assumed by constant efficiency, and a lumped parameter model is used to describe solar receiver including energy losses of conduction and reradiation. This framework also allows us to provide design guidelines for PTEC devices with high solar-to-electricity (STE) efficiency and solar-to-hydrogen (STH) efficiency. The maximum STE and STH efficiency under reference conditions of PTEC device was found to be 4 % and 2 %. A further improved performance in terms of STE and STH efficiency are about 19 % and 16 %, respectively, via optimizing temperature configuration between HTC and LTC and material properties. It is also interesting to note that STH can reach higher than 80 % of STE at a large temperature difference, which shows a promising energy storage device by storing excessive electrical power in form of hydrogen. The main results show that the temperature of HTC and efficiency of heat exchange are key parameters to optimize PTEC efficiency. The performance of DC-DC convertor dominates STH efficiency. Besides, ionic conductivity of electrolyte can contribute to significantly expanding the operating current density range. The PTEC is a promising technology for solar energy conversion and storage as it is able to produce electricity and hydrogen in a single device. The solar conversion efficiency predicted with our numerical model supports that by optimizing the design and operational conditions, this technology can compete with existing solar fuel pathways. Figure 1
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