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Photoelectrochemistry of Ultrathin, Semitransparent, and Catalytic Gold Films Electrodeposited Epitaxially onto n-Silicon (111)
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2018-06-01 00:00:00 , DOI: 10.1021/acsami.8b06388 Qingzhi Chen 1 , Jay A. Switzer 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2018-06-01 00:00:00 , DOI: 10.1021/acsami.8b06388 Qingzhi Chen 1 , Jay A. Switzer 1
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An ultrathin, epitaxial Au layer was electrochemically deposited on n-Si(111) to form a Schottky junction that was used as the photoanode in a regenerative photoelectrochemical cell. Au serves as a semitransparent contact that both stabilizes n-Si against photopassivation and catalyzes the oxidation of Fe2+ to Fe3+. In this cell, Fe2+ was oxidized at the n-Si(111)/Au(111) photoanode and Fe3+ was reduced at the Au cathode, leading to the conversion of solar energy into electrical energy with no net chemical reaction. The photocurrent was limited to 11.9 mA·cm–2 because of the absorption of light by the Fe2+/3+ redox couple. When a transparent solution of sulfite ion was oxidized at the photoanode, photocurrent densities as high as 28.5 mA·cm–2 were observed with AM 1.5 light of 100 mW·cm–2 intensity. One goal of the work was to determine the effect of the Au layer on the interfacial energetics as a function of the Au coverage. There was a decrease in the barrier height from 0.81 to 0.73 eV as the gold coverage was increased from island growth with 10% coverage to a dense Au film with a thickness of 11 nm. In all cases, the band-bending in n-Si was induced by the n-Si/Au Schottky junction instead of the energetic mismatch between the Fermi level of n-Si and the redox couple. The dense Au film gave the greatest stability. Although the photocurrent of the n-Si/Au photoanode with 10.2% island coverage dropped nearly to zero within 2 h, the photocurrent of the photoanode with a dense 11 nm thick Au film only decreased to 92% of its initial value after irradiation at open circuit with AM 1.5 light for 16 h. A 2.1 nm thick layer of SiOx formed between the Au film and n-Si. With further irradiation, the fill factor decreased because of the increase of series resistance as the SiOx layer thickness exceeded tunneling dimensions.
中文翻译：
外延电沉积在正硅上的超薄，半透明和催化金膜的光电化学（111）
将超薄外延Au层电化学沉积在n-Si（111）上以形成肖特基结，该结用作再生光电化学电池中的光阳极。Au用作半透明接触，既可以稳定n-Si免受光钝化，又可以催化Fe 2+氧化为Fe 3+。在该电池中，Fe 2+在n-Si（111）/ Au（111）光电阳极上被氧化，Fe 3+在Au阴极上被还原，导致太阳能转化为电能，而没有净化学反应。由于Fe 2 + / 3 +对光的吸收，光电流被限制在11.9 mA·cm –2氧化还原夫妇。当亚硫酸根离子的透明溶液在光电阳极被氧化，光电流密度高达28.5毫安·厘米-2用AM1.5光100毫瓦进行观察·厘米-2强度。这项工作的一个目标是确定Au层对界面能学的影响作为Au覆盖率的函数。随着金的覆盖率从具有10％覆盖率的岛生长到厚度为11 nm的致密金膜增加，势垒高度从0.81 eV降低到0.73 eV。在所有情况下，n-Si中的能带弯曲都是由n-Si / Au肖特基结引起的，而不是由n-Si的费米能级和氧化还原对之间的能量失配引起的。致密的金膜具有最大的稳定性。尽管岛上覆盖率达10.2％的n-Si / Au光电阳极的光电流在2小时内几乎降至零，但具有11nm厚致密Au膜的光电阳极的光电流仅在敞开照射后降低至其初始值的92％。电路用AM 1.5灯照明16小时。2.1纳米厚的SiO层在金膜和n-Si之间形成x。随着进一步的照射，由于SiO x层厚度超过隧穿尺寸，串联电阻增加，填充因子降低。
更新日期：2018-06-01
中文翻译：
外延电沉积在正硅上的超薄，半透明和催化金膜的光电化学（111）
将超薄外延Au层电化学沉积在n-Si（111）上以形成肖特基结，该结用作再生光电化学电池中的光阳极。Au用作半透明接触，既可以稳定n-Si免受光钝化，又可以催化Fe 2+氧化为Fe 3+。在该电池中，Fe 2+在n-Si（111）/ Au（111）光电阳极上被氧化，Fe 3+在Au阴极上被还原，导致太阳能转化为电能，而没有净化学反应。由于Fe 2 + / 3 +对光的吸收，光电流被限制在11.9 mA·cm –2氧化还原夫妇。当亚硫酸根离子的透明溶液在光电阳极被氧化，光电流密度高达28.5毫安·厘米-2用AM1.5光100毫瓦进行观察·厘米-2强度。这项工作的一个目标是确定Au层对界面能学的影响作为Au覆盖率的函数。随着金的覆盖率从具有10％覆盖率的岛生长到厚度为11 nm的致密金膜增加，势垒高度从0.81 eV降低到0.73 eV。在所有情况下，n-Si中的能带弯曲都是由n-Si / Au肖特基结引起的，而不是由n-Si的费米能级和氧化还原对之间的能量失配引起的。致密的金膜具有最大的稳定性。尽管岛上覆盖率达10.2％的n-Si / Au光电阳极的光电流在2小时内几乎降至零，但具有11nm厚致密Au膜的光电阳极的光电流仅在敞开照射后降低至其初始值的92％。电路用AM 1.5灯照明16小时。2.1纳米厚的SiO层在金膜和n-Si之间形成x。随着进一步的照射，由于SiO x层厚度超过隧穿尺寸，串联电阻增加，填充因子降低。
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