Engineering Sub-Nanometer Hafnia-Based Ferroelectrics to Break the Scaling Relation for High-Efficiency Piezocatalytic Water Splitting,Advanced Materials

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Engineering Sub-Nanometer Hafnia-Based Ferroelectrics to Break the Scaling Relation for High-Efficiency Piezocatalytic Water Splitting
Advanced Materials ( IF 27.4 ) Pub Date : 2023-07-06 , DOI: 10.1002/adma.202303018
Ran Su ₁ , Jiahui Zhang ₁ , Vienna Wong ₂ , Dawei Zhang _{2,

3} , Yong Yang ₄ , Zheng-Dong Luo ₅ , Xiaojing Wang ₁ , Hui Wen ₆ , Yang Liu ₇ , Jan Seidel _{2,

3} , Xiaolong Yang ₈ , Ying Pan ₉ , Fa-Tang Li ₁

Affiliation

Hebei Key Laboratory of Photoelectric Control on Surface and Interface, College of Science, Hebei University of Science and Technology, Shijiazhuang, 050018, P. R. China.
School of Materials Science and Engineering, University of New South Wales Australia, Sydney, New South Wales, 2052, Australia.
ARC Centre of Excellence in Future Low-Energy Electronics Technologies, UNSW Sydney, Sydney, NSW, 2052, Australia.
State Key Laboratory of Solidification Processing, Center of Advanced Lubrication and Seal Materials, Northwestern Polytechnical University, Xi'an, 710072, P. R. China.
State Key Discipline Laboratory of Wide Band Gap Semiconductor Technology, School of Microelectronics, Xidian University, Xi'an, 710071, P. R. China.
College of Electrical Engineering, Hebei University of Science and Technology, Shijiazhuang, 050018, P. R. China.
School of Materials Science and Engineering, State Key Laboratory of Material Processing and Die & Mould Technology, Huazhong University of Science and Technology, Wuhan, 430074, P. R. China.
College of Physics & Chongqing Key Laboratory for Strongly Coupled Physics, Center of Quantum Materials and Devices, Chongqing University, Chongqing, 401331, P. R. China.
Department of Chemistry, University of Paderborn, 33098, Paderborn, Germany.

Reversible control of ferroelectric polarization is essential to overcome the heterocatalytic kinetic limitation. This can be achieved by creating a surface with switchable electron density; however, owing to the rigidity of traditional ferroelectric oxides, achieving polarization reversal in piezocatalytic processes remains challenging. Herein, sub-nanometer-sized Hf_0.5Zr_0.5O₂ (HZO) nanowires with a polymer-like flexibility are synthesized. Oxygen K-edge X-ray absorption spectroscopy and negative spherical aberration-corrected transmission electron microscopy reveal an orthorhombic (Pca2₁) ferroelectric phase of the HZO sub-nanometer wires (SNWs). The ferroelectric polarization of the flexible HZO SNWs can be easily switched by slight external vibration, resulting in dynamic modulation of the binding energy of adsorbates and thus breaking the “scaling relationship” during piezocatalysis. Consequently, the as-synthesized ultrathin HZO nanowires display superb water-splitting activity, with H₂ production rate of 25687 µmol g⁻¹ h⁻¹ under 40 kHz ultrasonic vibration, which is 235 and 41 times higher than those of non-ferroelectric hafnium oxides and rigid BaTiO₃ nanoparticles, respectively. More strikingly, the hydrogen production rates can reach 5.2 µmol g⁻¹ h⁻¹ by addition of stirring exclusively.

中文翻译：

工程亚纳米铪基铁电体打破高效压电催化水分解的比例关系

铁电极化的可逆控制对于克服异质催化动力学限制至关重要。这可以通过创建具有可切换电子密度的表面来实现；然而，由于传统铁电氧化物的刚性，在压电催化过程中实现极化反转仍然具有挑战性。在此，合成了具有聚合物样柔性的亚纳米尺寸的Hf _0.5 Zr _0.5 O _{2 (HZO)纳米线。}氧 K 边 X 射线吸收光谱和负球差校正透射电子显微镜揭示了HZO 亚纳米线 (SNW) 的正交晶系( Pca2 ₁ )铁电相。柔性HZO SNW的铁电极化可以通过轻微的外部振动轻松切换，从而动态调节吸附物的结合能，从而打破压电催化过程中的“缩放关系”。因此，所合成的超细HZO纳米线表现出优异的水分解活性，在40 kHz超声振动下H ₂产率达到25687 µmol g ^-1 h ^-1，分别是非铁电铪的235倍和41倍氧化物和刚性BaTiO ₃纳米粒子，分别。更引人注目的是，仅通过搅拌，氢气产率可以达到5.2 µmol g ^-1 h ^{-1 。}

更新日期：2023-07-06

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