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Yttrium-Doped ZnO Nanorod Arrays for Increased Charge Mobility and Carrier Density for Enhanced Solar Water Splitting
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2019-07-23 , DOI: 10.1021/acs.jpcc.9b03609 Daniel Commandeur 1 , Grant Brown 1 , Peter McNulty 1 , Christopher Dadswell 1 , John Spencer 1 , Qiao Chen 1
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2019-07-23 , DOI: 10.1021/acs.jpcc.9b03609 Daniel Commandeur 1 , Grant Brown 1 , Peter McNulty 1 , Christopher Dadswell 1 , John Spencer 1 , Qiao Chen 1
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An innovative procedure is presented, when for the first time, yttrium-doped ZnO vertically aligned nanorods (NRs) have been synthesized using a unique rapid microwave-assisted method. In comparison with pristine ZnO NRs, the Y-doped samples present a more favorable morphology along with reduced crystallinity because of substitutional defects, YZn. Y acted as a shallow donor-type defect, leading to an 80% increase in dopant density, to 1.36 × 1018 cm–2 in the 0.15% Y sample. The transmission line model was used to analyze the transport properties. It was found that a 1000-fold increase in conductivity and electron mobility was achieved by doping 0.15% Y, resulting in a high density of donors which fill charge traps. Meanwhile, a significant improvement in conductivity was accompanied by greater electron hole recombination and band gap reduction. The analysis of photoluminescence spectra reveals the effect of Y doping on native point defects, initially reducing Zn2+ vacancies by filling with YZn, followed by the reduction of O2– vacancies with interstitial doping at higher Y concentration. With a fine balance of superior conductivity and charge recombination rate, the photocatalytic water splitting performance was optimized, achieving a photocurrent of 0.84 mA cm–2 at 1.23 VRHE with 0.1% Y doping. This corresponded to a 47% enhancement in photoconversion efficiency compared to the pristine sample.
中文翻译：
钇掺杂的ZnO纳米棒阵列，用于提高电荷迁移率和载流子密度，以增强太阳能水的分解
提出了一种创新的方法，这是首次使用独特的快速微波辅助方法合成了掺钇的ZnO垂直排列的纳米棒（NRs）。与原始的ZnO NRs相比，掺Y的样品由于置换缺陷Y Zn呈现出更有利的形貌以及降低的结晶度。Y充当浅施主型缺陷，导致掺杂剂密度增加80％，达到1.36×10 18 cm –2在0.15％的Y样本中。传输线模型用于分析传输特性。发现通过掺杂0.15％的Y实现了电导率和电子迁移率的1000倍的增加，导致填充电荷陷阱的供体的高密度。同时，电导率的显着提高伴随着更大的电子空穴复合和带隙减小。光致发光光谱分析揭示了Y掺杂对本征点缺陷的影响，首先通过填充Y Zn来减少Zn 2+空位，然后减少O 2–在较高的Y浓度下存在间隙掺杂的空位。凭借优异的电导率和电荷复合率的良好平衡，优化了光催化水分解性能，在1.23 V RHE和0.1％Y掺杂下实现了0.84 mA cm –2的光电流。与原始样品相比，这相当于光转换效率提高了47％。
更新日期：2019-07-24
中文翻译：
钇掺杂的ZnO纳米棒阵列，用于提高电荷迁移率和载流子密度，以增强太阳能水的分解
提出了一种创新的方法，这是首次使用独特的快速微波辅助方法合成了掺钇的ZnO垂直排列的纳米棒（NRs）。与原始的ZnO NRs相比，掺Y的样品由于置换缺陷Y Zn呈现出更有利的形貌以及降低的结晶度。Y充当浅施主型缺陷，导致掺杂剂密度增加80％，达到1.36×10 18 cm –2在0.15％的Y样本中。传输线模型用于分析传输特性。发现通过掺杂0.15％的Y实现了电导率和电子迁移率的1000倍的增加，导致填充电荷陷阱的供体的高密度。同时，电导率的显着提高伴随着更大的电子空穴复合和带隙减小。光致发光光谱分析揭示了Y掺杂对本征点缺陷的影响，首先通过填充Y Zn来减少Zn 2+空位，然后减少O 2–在较高的Y浓度下存在间隙掺杂的空位。凭借优异的电导率和电荷复合率的良好平衡，优化了光催化水分解性能，在1.23 V RHE和0.1％Y掺杂下实现了0.84 mA cm –2的光电流。与原始样品相比，这相当于光转换效率提高了47％。
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