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Investigations of the stability of etched or platinized p-InP(100) photocathodes for solar-driven hydrogen evolution in acidic or alkaline aqueous electrolytes
Energy & Environmental Science ( IF 32.5 ) Pub Date : 2021-09-30 , DOI: 10.1039/d1ee02809j Weilai Yu 1 , Matthias H. Richter 1, 2 , Pakpoom Buabthong 2 , Ivan A. Moreno-Hernandez 1 , Carlos G. Read 1 , Ethan Simonoff 1 , Bruce S. Brunschwig 3 , Nathan S. Lewis 1, 3
Energy & Environmental Science ( IF 32.5 ) Pub Date : 2021-09-30 , DOI: 10.1039/d1ee02809j Weilai Yu 1 , Matthias H. Richter 1, 2 , Pakpoom Buabthong 2 , Ivan A. Moreno-Hernandez 1 , Carlos G. Read 1 , Ethan Simonoff 1 , Bruce S. Brunschwig 3 , Nathan S. Lewis 1, 3
Affiliation
The stability of p-InP photocathodes performing the hydrogen-evolution reaction (HER) has been evaluated in contact with either 1.0 M H2SO4(aq) or 1.0 M KOH(aq), with a focus on identifying corrosion mechanisms. Stability for the solar-driven HER was evaluated using p-InP electrodes that were either etched or coated with an electrodeposited Pt catalyst (p-InP/Pt). Variables such as trace O2 were systematically controlled during the measurements. Changes in surface characteristics after exposure to electrochemical conditions as well as electrode dissolution processes were monitored using X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma mass spectrometry (ICP-MS). In either H2SO4 or KOH, etched p-InP photoelectrodes corroded cathodically under illumination, forming metallic In0 at the electrode surface. In contrast, electrodeposition of Pt kinetically stabilized illuminated p-InP photocathodes in both H2SO4 and KOH by inhibiting the cathodic corrosion pathway. Notably, when held at 0 V vs. the reversible hydrogen electrode (RHE) in 1.0 M H2SO4(aq), p-InP/Pt exhibited a stable current density (J) of ∼−18 mA cm−2 for >285 h under simulated 1 Sun illumination. The long-term current density vs. potential (J–E) behavior at pH 0 and pH 14 of p-InP/Pt photocathodes correlated with changes in the surface chemistry as well as the dissolution of p-InP. In acidic media, the J–E behavior of p-InP/Pt photocathodes remained nearly constant with time, but the surface of a p-InP/Pt electrodes gradually turned P-rich via a slow and continuous leaching of In ions. In alkaline electrolyte, the surface of p-InP/Pt electrodes was passivated by formation of an InOx layer that exhibited negligible dissolution but led to a substantial degradation in the J–E characteristics. Consequently, changes in the catalytic kinetics and surface stoichiometry are both important considerations for determining the corrosion chemistry and the long-term operational stability of InP photoelectrodes.
中文翻译:
酸性或碱性水性电解质中用于太阳能驱动析氢的蚀刻或镀铂 p-InP(100) 光电阴极稳定性的研究
进行析氢反应 (HER) 的 p-InP 光电阴极的稳定性已通过与 1.0 MH 2 SO 4 (aq) 或 1.0 M KOH(aq)接触进行评估,重点是确定腐蚀机制。太阳能驱动 HER 的稳定性使用 p-InP 电极进行评估,这些电极经过蚀刻或涂有电沉积 Pt 催化剂 (p-InP/Pt)。在测量过程中系统地控制了诸如痕量 O 2 之类的变量。使用 X 射线光电子能谱 (XPS) 和电感耦合等离子体质谱 (ICP-MS) 监测暴露于电化学条件以及电极溶解过程后表面特性的变化。在 H 2 SO 4或 KOH,蚀刻的 p-InP 光电极在光照下发生阴极腐蚀,在电极表面形成金属 In 0。相比之下,Pt 的电沉积通过抑制阴极腐蚀途径在 H 2 SO 4和 KOH 中稳定地照射 p-InP 光电阴极。值得注意的是,当在 1.0 MH 2 SO 4 (aq) 中相对于可逆氢电极 (RHE)保持在 0 V 时,p-InP/Pt 表现出稳定的电流密度 ( J ) 为~-18 mA cm -2 >285 h 在模拟 1 日照度下。长期电流密度与电位 ( J – E) p-InP/Pt 光电阴极在 pH 0 和 pH 14 下的行为与表面化学变化以及 p-InP 的溶解相关。在酸性介质中,p-InP/Pt 光电阴极的J - E行为随时间几乎保持不变,但 p-InP/Pt 电极的表面通过In 离子的缓慢和连续浸出逐渐变成富 P。在碱性电解质中,p-InP/Pt 电极的表面通过形成 InO x层而钝化,该层表现出可忽略不计的溶解,但导致J - E的显着降解特征。因此,催化动力学和表面化学计量的变化都是确定 InP 光电极的腐蚀化学和长期运行稳定性的重要考虑因素。
更新日期:2021-10-14
中文翻译:
酸性或碱性水性电解质中用于太阳能驱动析氢的蚀刻或镀铂 p-InP(100) 光电阴极稳定性的研究
进行析氢反应 (HER) 的 p-InP 光电阴极的稳定性已通过与 1.0 MH 2 SO 4 (aq) 或 1.0 M KOH(aq)接触进行评估,重点是确定腐蚀机制。太阳能驱动 HER 的稳定性使用 p-InP 电极进行评估,这些电极经过蚀刻或涂有电沉积 Pt 催化剂 (p-InP/Pt)。在测量过程中系统地控制了诸如痕量 O 2 之类的变量。使用 X 射线光电子能谱 (XPS) 和电感耦合等离子体质谱 (ICP-MS) 监测暴露于电化学条件以及电极溶解过程后表面特性的变化。在 H 2 SO 4或 KOH,蚀刻的 p-InP 光电极在光照下发生阴极腐蚀,在电极表面形成金属 In 0。相比之下,Pt 的电沉积通过抑制阴极腐蚀途径在 H 2 SO 4和 KOH 中稳定地照射 p-InP 光电阴极。值得注意的是,当在 1.0 MH 2 SO 4 (aq) 中相对于可逆氢电极 (RHE)保持在 0 V 时,p-InP/Pt 表现出稳定的电流密度 ( J ) 为~-18 mA cm -2 >285 h 在模拟 1 日照度下。长期电流密度与电位 ( J – E) p-InP/Pt 光电阴极在 pH 0 和 pH 14 下的行为与表面化学变化以及 p-InP 的溶解相关。在酸性介质中,p-InP/Pt 光电阴极的J - E行为随时间几乎保持不变,但 p-InP/Pt 电极的表面通过In 离子的缓慢和连续浸出逐渐变成富 P。在碱性电解质中,p-InP/Pt 电极的表面通过形成 InO x层而钝化,该层表现出可忽略不计的溶解,但导致J - E的显着降解特征。因此,催化动力学和表面化学计量的变化都是确定 InP 光电极的腐蚀化学和长期运行稳定性的重要考虑因素。