High performance III-V photoelectrodes for solar water splitting via synergistically tailored structure and stoichiometry
High performance III-V photoelectrodes for solar water splitting via synergistically tailored structure and stoichiometry
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DOI：
10.1038/s41467-019-11351-1
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发表时间：
2019-07-29
影响因子：
16.6
通讯作者：
Yoon, Jongseung
中科院分区：
文献类型：
--
作者：
Lim, Haneol;Young, James L.;Yoon, Jongseung
半导体光电极的催化界面具有光吸收、电催化和防腐蚀等多重作用，是高效光电化学太阳能水分解的关键。然而，同时优化这些过程中的每一个代表了材料的难题，由于在电极表面的材料属性的相互冲突的要求。在这里，我们展示了一种方法，可以规避这些挑战，协同利用耐腐蚀表面化学计量和结构定制的反应界面。纳米多孔，密度梯度表面的“黑色”磷化铟镓（GaInP2），当结合硫化铵为基础的表面钝化，有效地减少反射和表面复合的光生载流子的高效率抑制在析氢半反应，但也增加了电化学耐久性与寿命超过124小时通过强烈抑制腐蚀动力学。这种化学计量和反应界面处的结构的协同控制提供了一种实用的途径，以同时提高半导体光电极的效率和耐久性，而不仅仅依赖于新的保护材料的开发。
Catalytic interface of semiconductor photoelectrodes is critical for high-performance photoelectrochemical solar water splitting because of its multiple roles in light absorption, electrocatalysis, and corrosion protection. Nevertheless, simultaneously optimizing each of these processes represents a materials conundrum owing to conflicting requirements of materials attributes at the electrode surface. Here we show an approach that can circumvent these challenges by collaboratively exploiting corrosion-resistant surface stoichiometry and structurally-tailored reactive interface. Nanoporous, density-graded surface of 'black' gallium indium phosphide (GaInP2), when combined with ammonium-sulfide-based surface passivation, effectively reduces reflection and surface recombination of photogenerated carriers for high efficiency photocatalysis in the hydrogen evolution half-reaction, but also augments electrochemical durability with lifetime over 124 h via strongly suppressed kinetics of corrosion. Such synergistic control of stoichiometry and structure at the reactive interface provides a practical pathway to concurrently enhance efficiency and durability of semiconductor photoelectrodes without solely relying on the development of new protective materials.