Tuning Bifunctional Oxygen Electrocatalysts by Changing the A-Site Rare-Earth Element in Perovskite Nickelates

Wang Le; Stoerzinger Kelsey A.; Chang Lei; Zhao Jiali; Li Yangyang; Tang Chi Sin; Yin Xinmao; Bowden Mark E.; Yang Zhenzhong; Guo Haizhong; You Lu; Guo Rui; Wang Jiaou; Ibrahim Kurash; Chen Jingsheng; Rusydi Andrivo; Wang Junling; Chambers Scott A.; Du Yingge

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Tuning Bifunctional Oxygen Electrocatalysts by Changing the A-Site Rare-Earth Element in Perovskite Nickelates

机译：通过改变钙钛矿型镍酸盐中的A-位稀土元素来调节双功能氧电催化剂

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Perovskite-structured (ABO(3)) transition metal oxides are promising bifunctional electrocatalysts for efficient oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). In this paper, a set of epitaxial rare-earth nickelates (RNiO3) thin films is investigated with controlled A-site isovalent substitution to correlate their structure and physical properties with ORR/OER activities, examined by using a three-electrode system in O-2-saturated 0.1 m KOH electrolyte. The ORR activity decreases monotonically with decreasing the A-site element ionic radius which lowers the conductivity of RNiO3 (R = La, La0.5Nd0.5, La0.2Nd0.8, Nd, Nd0.5Sm0.5, Sm, and Gd) films, with LaNiO3 being the most conductive and active. On the other hand, the OER activity initially increases upon substituting La with Nd and is maximal at La0.2Nd0.8NiO3. Moreover, the OER activity remains comparable within error through Sm-doped NdNiO3. Beyond that, the activity cannot be measured due to the potential voltage drop across the film. The improved OER activity is ascribed to the partial reduction of Ni3+ to Ni2+ as a result of oxygen vacancies, which increases the average occupancy of the e(g) antibonding orbital to more than one. The work highlights the importance of tuning A-site elements as an effective strategy for balancing ORR and OER activities of bifunctional electrocatalysts.

机译：钙钛矿结构的（ABO（3））过渡金属氧化物是有前途的双功能电催化剂，可用于有效的氧释放反应（OER）和氧还原反应（ORR）。本文研究了一组外延稀土镍酸盐（RNiO3）薄膜，这些薄膜具有受控的A-位等价取代，以将其结构和物理性质与ORR / OER活性相关联，并在O-中使用三电极系统进行了研究2饱和的0.1 m KOH电解质。 ORR活性随A位元素离子半径的减小而单调降低，从而降低RNiO3的电导率（R = La，La0.5Nd0.5，La0.2Nd0.8，Nd，Nd0.5Sm0.5，Sm和Gd） LaNiO3是最导电和最活跃的薄膜。另一方面，在用La代替La时，OER活性最初会增加，在La0.2Nd0.8NiO3处最大。此外，通过掺Sm的NdNiO3，OER活性在误差范围内仍然相当。除此之外，由于膜上的潜在电压降，无法测量活性。 OER活性的提高归因于氧空位导致Ni3 +部分还原为Ni2 +，这将e（g）反键轨道的平均占有率提高到一个以上。这项工作强调了调整A位元素作为平衡双功能电催化剂ORR和OER活性的有效策略的重要性。

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来源
《Advanced Functional Materials》 |2018年第39期|1803712.1-1803712.8|共8页
作者
Wang Le; Stoerzinger Kelsey A.; Chang Lei; Zhao Jiali; Li Yangyang; Tang Chi Sin; Yin Xinmao; Bowden Mark E.; Yang Zhenzhong; Guo Haizhong; You Lu; Guo Rui; Wang Jiaou; Ibrahim Kurash; Chen Jingsheng; Rusydi Andrivo; Wang Junling; Chambers Scott A.; Du Yingge;
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作者单位

Pacific Northwest Natl Lab, Phys & Computat Sci Directorate, Richland, WA 99354 USA;

Pacific Northwest Natl Lab, Phys & Computat Sci Directorate, Richland, WA 99354 USA;

Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore;

Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100039, Peoples R China;

Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore;

Natl Univ Singapore, NUS Grad Sch Integrat Sci & Engn, Singapore 117456, Singapore;

Natl Univ Singapore, Fac Sci, Dept Phys, Singapore 117542, Singapore;

Pacific Northwest Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA;

Pacific Northwest Natl Lab, Phys & Computat Sci Directorate, Richland, WA 99354 USA;

Zhengzhou Univ, Sch Phys Engn, Zhengzhou 450001, Henan, Peoples R China;

Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore;

Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore;

Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100039, Peoples R China;

Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100039, Peoples R China;

Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore;

Natl Univ Singapore, Fac Sci, Dept Phys, Singapore 117542, Singapore;

Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore;

Pacific Northwest Natl Lab, Phys & Computat Sci Directorate, Richland, WA 99354 USA;

Pacific Northwest Natl Lab, Phys & Computat Sci Directorate, Richland, WA 99354 USA;

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正文语种 eng
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关键词
nickelates; oxygen evolution reaction; oxygen reduction reaction; oxygen vacancy; perovskite;

机译：镍酸盐;析氧反应;氧还原反应;氧空位;钙钛矿;

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机译：A现场掺杂的钙钛矿氧化物强烈的界面与碳纳米管耦合，作为用于固态Zn空气电池的有前途的双官能电催化剂
3. Carbon-based lanthanum nickelate material La2-x-yNdxPryNiO4+delta (x=0, 0.3, and 0.5; y=0 and 0.2) as a bifunctional electrocatalyst for oxygen reduction in alkaline media [J] . Amira Sabah, Ferkhi Mosbah, Khaled Ammar, Ionics . 2019,第8期

机译：基于碳的镧镍材料La2-X-YNDXPRYNIO4 +δ（x = 0,0.3和0.5; y = 0和0.2），作为碱性介质的氧还原的双功能电催化剂
4. Pressure-induced Valence Change of Rare-earth and Transition Elements in Perovskite Oxides [C] . Wenhui Su, Liping Li, Jipeng Miao, Third China-Japan High Pressure Seminar April 5-9, 1998 Chengdu, China . 1998

机译：钙钛矿氧化物中稀土和过渡元素的压力诱导化合价变化
5. Tuning Structural and Physical Properties via A-Site Doping in Perovskite-Type Transition Metal Oxides [D] . Somaily, Hamoud H. 2018

机译：通过钙钛矿型过渡金属氧化物中的A站点掺杂来调整结构和物理性质
6. A-Site Cation-Ordering Layered Perovskite EuBa0.5Sr0.5Co2–xFexO5+δ as Highly Activeand Durable Electrocatalysts for Oxygen Evolution Reaction [O] . Xiu Wang, Yingnan Dou, Ying Xie, 2020

机译：高活性的A站点阳离子有序分层钙钛矿EuBa0.5Sr0.5Co2–xFexO5 +δ和耐用的氧析出反应电催化剂
7. Tuning Photovoltaic Performance of Perovskite Nickelates Heterostructures by Changing the ASite Rare-Earth Element [O] . -1

机译：通过改变稀土元素改变钙钛矿钙钛矿异质结构的光伏性能

Tuning Bifunctional Oxygen Electrocatalysts by Changing the A-Site Rare-Earth Element in Perovskite Nickelates

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