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Atomic Layer Deposited TiO2–IrOx Alloys Enable Corrosion Resistant Water Oxidation on Silicon at High Photovoltage
Chemistry of Materials ( IF 7.2 ) Pub Date : 2018-12-10 00:00:00 , DOI: 10.1021/acs.chemmater.8b03092 Olivia L. Hendricks 1 , Robert Tang-Kong 2 , Aein S. Babadi 2 , Paul C. McIntyre 2 , Christopher E. D. Chidsey 1
Chemistry of Materials ( IF 7.2 ) Pub Date : 2018-12-10 00:00:00 , DOI: 10.1021/acs.chemmater.8b03092 Olivia L. Hendricks 1 , Robert Tang-Kong 2 , Aein S. Babadi 2 , Paul C. McIntyre 2 , Christopher E. D. Chidsey 1
Affiliation
We synthesized by atomic layer deposition (ALD) TiO2–IrOx alloys that enable high photovoltages and catalyze water oxidation on silicon metal–insulator–semiconductor (MIS) photoanodes. The ratio of TiO2 to IrOx was precisely controlled by varying the number of ALD cycles for each precursor. Silicon with a 2 nm surface SiO2 layer was coated with TiO2–IrOx alloys ranging in composition from 18 to 35% iridium relative to the sum of titanium and iridium concentrations. IrOx catalyzed oxygen evolution and imparted a high work function to the TiO2–IrOx alloys, enabling photovoltages during water oxidation that exceeded 600 mV. TiO2 imparted stability and inhibited corrosion of the underlying silicon light absorber. After annealing in forming gas (5% H2/95% N2), TiO2–IrOx alloys were stable for 12 h of continuous water oxidation in 1 M H2SO4. Key properties of the MIS junction affecting electrochemical operation were also extracted by electrochemical impedance spectroscopy. This work demonstrates that alloying by ALD is a promising approach for designing corrosion resistant Schottky contacts with optimized electronic and materials properties for catalyzed, solar driven water oxidation.
中文翻译:
原子层沉积的TiO 2 -IrO x合金可在高光电压下在硅上实现耐腐蚀的水氧化
我们通过原子层沉积(ALD)TiO 2 -IrO x合金进行合成,这些合金能够在硅金属-绝缘体-半导体(MIS)光电阳极上实现高光电压并催化水氧化。通过改变每种前体的ALD循环数来精确地控制TiO 2与IrO x的比率。用TiO 2 -IrO x合金涂覆具有2 nm表面SiO 2层的硅,其成分相对于钛和铱浓度的总和为18%至35%的铱。IrO x催化氧的释放并赋予TiO 2 -IrO x高功函数合金,使水氧化过程中的光电压超过600 mV。TiO 2赋予了稳定性并抑制了下面的硅光吸收剂的腐蚀。在形成气体(5%H 2 /95%N 2)中退火后,TiO 2 -IrO x合金在1 MH 2 SO 4中连续水氧化12小时稳定。还通过电化学阻抗谱提取了MIS结影响电化学操作的关键特性。这项工作表明,通过ALD合金化是设计具有优化的电子和材料性能以催化太阳能驱动的水氧化的耐腐蚀肖特基接触的一种有前途的方法。
更新日期:2018-12-10
中文翻译:
原子层沉积的TiO 2 -IrO x合金可在高光电压下在硅上实现耐腐蚀的水氧化
我们通过原子层沉积(ALD)TiO 2 -IrO x合金进行合成,这些合金能够在硅金属-绝缘体-半导体(MIS)光电阳极上实现高光电压并催化水氧化。通过改变每种前体的ALD循环数来精确地控制TiO 2与IrO x的比率。用TiO 2 -IrO x合金涂覆具有2 nm表面SiO 2层的硅,其成分相对于钛和铱浓度的总和为18%至35%的铱。IrO x催化氧的释放并赋予TiO 2 -IrO x高功函数合金,使水氧化过程中的光电压超过600 mV。TiO 2赋予了稳定性并抑制了下面的硅光吸收剂的腐蚀。在形成气体(5%H 2 /95%N 2)中退火后,TiO 2 -IrO x合金在1 MH 2 SO 4中连续水氧化12小时稳定。还通过电化学阻抗谱提取了MIS结影响电化学操作的关键特性。这项工作表明,通过ALD合金化是设计具有优化的电子和材料性能以催化太阳能驱动的水氧化的耐腐蚀肖特基接触的一种有前途的方法。