Sustainable Energy Conversion Systems Research Articles

Performance evaluation of an open-cathode PEM fuel cell stack under ambient conditions: Case study of United Arab Emirates

The open-cathode polymer electrolyte membrane (PEM) fuel cell stack has been a promising candidate as a sustainable energy conversion system for replacing fossil fuel-based energy conversion devices in portable and automotive applications. As the ambient air is directly used to provide both oxidant and cooling, the complex cooling loop can be avoided which reduces the complexity and cost. However, the stack performance is highly affected by ambient conditions, i.e., ambient temperature and humidity. In this study, the effect of monthly ambient air conditions (temperature and humidity) is evaluated with respect to the stack’s power production performance as well as thermal, water and gas management by employing a validated three-dimensional open-cathode PEM fuel cell stack model. The annual climate data from the hot and arid environment of Abu Dhabi, United Arab Emirates (UAE) are used as a case study. The objective is to develop a better fundamental understanding of the interactions of physical phenomena in a fuel cell stack, which can assist in improving the performance and operation of an open-cathode PEM fuel cell-powered vehicle. The results indicate that the stack performance can vary significantly (up to 40%) from winter to summer, especially at high operating currents, with significant changes in the stack temperature and the water content at the membrane. Moreover, the anode humidification results in a significant improvement in the stack performance (up to 40%) in hot and dry conditions. However, a careful balance has to be struck between the humidifier parasitic load and the stack power.

A CNT@MoSe2 hybrid catalyst for efficient and stable hydrogen evolution.

Exploration of high-efficiency Pt-free electrochemical catalysts for hydrogen evolution reaction (HER) is considered as a great challenge for the development of sustainable and carbon dioxide free energy conversion systems. In this work, a unique hierarchical nanostructure of few-layered MoSe2 nanosheets perpendicularly grown on carbon nanotubes (CNTs) is synthesized through a one-step solvothermal reaction. This rationally designed architecture based on a highly conductive CNT substrate possesses fully exposed active edges and open structures for fast ion/electron transfer, thus leading to remarkable HER activity with a low onset potential of -0.07 V vs. RHE (reversible hydrogen electrode), a small Tafel slope of 58 mV per decade and excellent long-cycle stability. Therefore, this noble-metal-free and highly efficient catalyst enables prospective applications for industrial, renewable hydrogen production.

Design of mononuclear ruthenium catalysts for low-overpotential water oxidation.

Water oxidation is a key reaction in natural photosynthesis and in many schemes for artificial photosynthesis. Inspired by energy challenges and the emerging understanding of photosystem II, the development of artificial molecular catalysts for water oxidation has become a highly active area of research in recent years. In this Focus Review, we describe recent achievements in the development of single-site ruthenium catalysts for water oxidation with a particular focus on the overpotential of water oxidation. First, we introduce the general scheme to access the high-valent ruthenium-oxo species, the key species of the water-oxidation reaction. Next, the mechanisms of the OO bond formation from the active ruthenium-oxo species are described. We then discuss strategies to decrease the onset potentials of the water-oxidation reaction. We hope this Focus Review will contribute to the further development of efficient catalysts toward sustainable energy-conversion systems.

Homogeneous photochemical water oxidation by biuret-modified Fe-TAML: evidence of Fe(V)(O) intermediate.

Water splitting, leading to hydrogen and oxygen in a process that mimics natural photosynthesis, is extremely important for devising a sustainable solar energy conversion system. Development of earth-abundant, transition metal-based catalysts that mimic the oxygen-evolving complex of photosystem II, which is involved in oxidation of water to O2 during natural photosynthesis, represents a major challenge. Further, understanding the exact mechanism, including elucidation of the role of active metal-oxo intermediates during water oxidation (WO), is critical to the development of more efficient catalysts. Herein, we report Fe(III) complexes of biuret-modified tetra-amidomacrocyclic ligands (Fe-TAML; 1a and 1b) that catalyze fast, homogeneous, photochemical WO to give O2, with moderate efficiency (maximum TON = 220, TOF = 0.76 s(-1)). Previous studies on photochemical WO using iron complexes resulted in demetalation of the iron complexes with concomitant formation of iron oxide nanoparticles (NPs) that were responsible for WO. Herein, we show for the first time that a high valent Fe(V)(O) intermediate species is photochemically generated as the active intermediate for the oxidation of water to O2. To the best of our knowledge, this represents the first example of a molecular iron complex catalyzing photochemical WO through a Fe(V)(O) intermediate.