Chlorophyll/Cu2O Heterostructure Leads to Increased Applied Bias Photon-to-Current Efficiency toward Enhanced Water Splitting

Yu-Teng Wu, Amit Kumar Sharma, Fei Pan* and Yen-Hsun Su*, 
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Abstract

The ongoing climate change and global warming urge quick replacement of fossil fuels and demand innovative strategies for clean energy generation energy. The solar-induced photoelectrochemical water splitting mechanism holds immense potential for hydrogen generation through metal oxide photocatalysts. However, poor visible light absorption, aqueous instability, electrode degradation, and exciton recombination are major hurdles to its application. To address these challenges, we have employed p-type cuprous oxide (Cu2O) electrodeposited on a conducting indium tin oxide (ITO) substrate to form a photoanode. The electrode was characterized systematically for its physicochemical and electrical properties. To facilitate solar to hydrogen conversion and enhance durability, we modified the electrode surface with chlorophyll. Owing to chlorophyll’s exceptional visible light absorption characteristics, the chlorophyll-modified Cu2O electrode exhibited a remarkably high photocurrent density (3.26 mA/cm2) and energy conversion, yielding a 0.82% to 1.37% increase in the applied bias photon-to-current efficiency (ABPE %). Furthermore, density of states calculations validated the bonding interactions between Mg (chlorophyll) and O (Cu2O) at the heterojunction. The electrode stabilities during the electrochemical reaction and post-electrochemical reaction were also compared, showing its potential applicability for hydrogen generation.

Abstract Image

叶绿素/Cu2O异质结构导致增加的应用偏压光子-电流效率,以增强水分裂
持续的气候变化和全球变暖促使化石燃料的快速替代,并要求清洁能源生产能源的创新战略。太阳能诱导的光电化学水分解机制在金属氧化物光催化剂制氢方面具有巨大的潜力。然而,可见光吸收差、水不稳定性、电极降解和激子复合是其应用的主要障碍。为了解决这些挑战,我们采用p型氧化亚铜(Cu2O)电沉积在导电氧化铟锡(ITO)衬底上形成光阳极。对该电极的理化性能和电学性能进行了系统的表征。为了促进太阳能到氢的转化和提高耐用性,我们用叶绿素修饰了电极表面。由于叶绿素独特的可见光吸收特性,叶绿素修饰的Cu2O电极表现出非常高的光电流密度(3.26 mA/cm2)和能量转换,使应用偏压光子电流效率(ABPE %)提高0.82%至1.37%。此外,态密度计算验证了Mg(叶绿素)和O (Cu2O)在异质结处的成键相互作用。比较了电极在电化学反应中和电化学反应后的稳定性,显示了其在制氢方面的潜在适用性。
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