Development Status of Textured Piezoelectric Ceramics and Preparation Processes

Round 1

Reviewer 1 Report

Comments and Suggestions for Authors

The manuscript proposes a review dedicated to factors that determine the performance parameters of piezoelectric ceramics, especially the preparation process of ceramics, which plays a decisive role in their properties.

The review presents an actual and interesting topic. However, the introduction is missing a series of very good quality international articles (e.g. European) dedicated to this topic, and therefore, I recommend improving the area from which the references are collected in order to obtain a more pertinent overview.

The data included in the review are coherent and present an attractive topic: the process flow of the texturing technique and the development of the application of the texturing process in the field of high-performance piezoelectric ceramics in recent years. The manuscript Included also the challenges and prospects of ceramic fabrication processes.

However, the manuscript text and images show multiple text editing errors (missing spaces, incorrect words, etc.). Detailed revision is recommended to meet the journal's requirements ( for example – figure 3 includes incorrect words – “magnetic”, overlaying text over images, missing spaces, etc.).

Conclusions can be improved with highlit on methods to achieving high-performance piezoelectric ceramics.

In conclusion, the reviewer considers that the presented version of the manuscript can be considered for publication in Coatings journal only with a major revision of the manuscript. 

Author Response

Comment 1:

1. The introduction is missing a series of very good quality international articles (e.g. European) dedicated to this topic, and therefore, I recommend improving the area from which the references are collected in order to obtain a more pertinent overview.

Response:

Thank you for your comments. The introduction of this article mainly discusses the development background and significance of textured ceramics. The references are adjusted as follows:

• Liu H, Li X, et al. Research progress in the study of textured piezoelectric ceramics[J]. Materials Science and Technology, 2024.
• Saito, H. Takao, T. Tani, T. et al , Lead-free piezoceramics[J]. Nature. 2004, 432: 84–87.
• Jinglei Li, Wanbo Qu, John Danielset,et al ,Lead zirconate titanate ceramics with aligned crystallite grains[J]. Science 380, 87–93 (2023).
• Zhang Y, Yu Y, Zhang N, et al. Simultaneous Realization of Good Piezoelectric and Strain Temperature Stability via the Synergic Contribution from Multilayer Design and Rare Earth Doping[J]. Advanced Functional Materials, 2023, 33(11): 2211439.
• RAMACHANDRAN V P,THOMAS DVINOD Tk.Design and development of a broadband spherical hydrophone using PZT-4[J]. ISSS Journal of Micro and Smart Systems2020,9(2):163-171.
• Wang, Q., Bian, L., Li, K., Liu, Y. C., Yang, Y. L., Yang, B., & Cao, W. Achieving ultrahigh electromechanical properties with high TC in PNN-PZT textured ceramics. Journal of Materials Science & Technology, 2024,175, 258-265.
• Lu G, Zhao Y, Zhao R, et al. High performance (K, Na) NbO₃-based textured ceramics for piezoelectric energy harvesting[J]. Ceramics International, 2024.
• Tian, Fenghua, et al. "Research on the Characteristics of High-Performance Textured Ceramic Materials and Their Application in Composite Rod Transducers." Actuators. Vol. 13. No. 11. MDPI, 2024.
• Zhao, Lianzhong, et al. "Three-dimensional honeycomb structured BaTiO₃-based piezoelectric ceramics via texturing and vat photopolymerization." Additive Manufacturing 95 (2024): 104542.
• Hu Z , Zhang H , Zhu Z ,et al.Deciphering the peculiar hysteresis loops of 0.05Pb(Mn_1/3Sb_2/3)O₃–0.95Pb(Zr₅₂Ti_0.48)O₃ piezoelectric ceramics[J].Acta materialia, 2023.
• van der Veer E, Noheda B, Acuautla M. Piezoelectric properties of PZT by an ethylene glycol-based chemical solution synthesis[J]. Journal of Sol-Gel Science and Technology, 2021, 100: 517-525.
• Chen J X, Li J W, Cheng C, et al. Piezoelectric property enhancement of PZT/Poly (vinylidenefluoride-co-trifluoroethylene) hybrid films for flexible piezoelectric energy harvesters[J]. ACS omega, 2021, 7(1): 793-803.
• Wang J , Wang S , Li X ,et al.High piezoelectricity and low strain hysteresis in PMN-PT-based piezoelectric ceramics[J].Advanced Ceramics, 2023, 12(4):11.
• Tian F, Liu Y, Ma R, et al. Properties of PMN-PT single crystal piezoelectric material and its application in underwater acoustic transducer[J]. Applied Acoustics, 2021, 175: 107827.
• Lv P, Qian J, Yang C, et al. Flexible all-inorganic Sm-doped PMN-PT film with ultrahigh piezoelectric coefficient for mechanical energy harvesting, motion sensing, and human-machine interaction[J]. Nano Energy, 2022, 97: 107182.
• Zu D , Zhang Y , Li H ,et al.Sintering pressure of SPS-inducing lattice deformation enhances ferroelectric and photoluminescence properties of PLZT ceramics[J].Journal of Materials Research, 2023, 38(11):2894-2907.
• Shcheglova, A.I., Kislova, I.L., Ilina, T.S. et al. Dielectric and Piezoelectric Properties of PLZT x/40/60 (x = 5; 12) Ceramics. Russ Microelectron 50, 673–678 (2021).
• Chen J , Zhou C , Liu H ,et al.Advances in mitigating the Td-d₃₃ trade-off via compositionally graded diffusion in BNT-based piezoceramic[J].Journal of the European Ceramic Society, 2023, 43(5):1923-1931.
• Wang Y, Wang P, Liu L, et al. Defect Dipole Behaviors on the Strain Performances of Bismuth Sodium Titanate-Based Lead-Free Piezoceramics[J]. Materials, 2023, 16(11): 4008.
• Viola G , Tian Y , Yu C ,et al.Electric field-induced transformations in bismuth sodium titanate-based materials[J].Progress in Materials Science, 2021:100837.
• A X Z , A G X , A H L ,et al.Phase Structure and Properties of Sodium Bismuth Titanate Lead-free Piezoelectric Ceramics[J].Progress in Materials Science, 2021.
• Dinh T H , Han H S , Tran V D N ,et al.Thermally-Stable High EFIS Properties of Ternary Lead-Free BNT-BKT-BZ Piezoelectric Ceramics[J].Journal of Electronic Materials, 2023.
• Liu Y, Khanbareh H, Halim M A, et al. Piezoelectric energy harvesting for self‐powered wearable upper limb applications[J]. Nano Select, 2021, 2(8): 1459-1479.
• Gao XY, Cheng ZX, Chen ZB, et al. The mechanism for the enhanced piezoelectricity in multi-elements doped (K,Na)NbO₃ Nat Commun 2021, 12: 881.
• Xu L, Lin J, Yang Y, et al. Ultrahigh thermal stability and piezoelectricity of lead-free KNN-based texture piezoceramics[J]. Nature Communications, 2024, 15(1): 9018.
• Bian L, Wang Q, He S, et al. Excellent strain and temperature stability in PNT-PZT multilayer textured ceramics[J]. Journal of the European Ceramic Society, 2024, 44(8): 5048-5054.
• Kim J S, Lee G S, Kim S H, et al. Effect of crystal structure on the improvement of the piezoelectric properties for [001]-textured PZT-PNN piezoceramics[J]. Ceramics International, 2024, 50(13): 23232-23243.
• Yin, J., Shi, X., Tao, H. et al. Deciphering the atomic-scale structural origin for large dynamic electromechanical response in lead-free Bi₅Na_0.5TiO₃-based relaxor ferroelectrics. Nat Commun 13, 6333 (2022).
• Wang Q, Bian L, Li K, et al. Achieving ultrahigh electromechanical properties with high TC in PNN-PZT textured ceramics[J]. Journal of Materials Science & Technology, 2024, 175: 258-265.
• Jia P , Zheng Z , Li Y ,et al.The achieving enhanced piezoelectric performance of KNN-based ceramics: Decisive role of multi-phase coexistence induced by lattice distortion[J].Journal of Alloys and Compounds: An Interdisciplinary Journal of Materials Science and Solid-state Chemistry and Physics, 2023.
• Wang B,Wang J,Li J,et al.Structure and electrical properties of La₂O₃-doped (K,Na,Li)(Nb,Ta)O₃-(Bi,Na)TiO₃ceramics[J].Journal of Advanced Dielectrics, 2023, 13(02).
• Zhao C , Huang Y , Wu J .Multifunctional barium titanate ceramics via chemical modification tuning phase structure[J].InfoMat, 2020(12).

    Comment 2:  

2. The manuscript text and images show multiple text editing errors (missing spaces, incorrect words, etc.)

Response:

Thank you for your comments.The formatting issues are modified as follows.

72:... believed that the higher the Tc, the higher its us...

84:...this segment to E=0, the intersection ...

105:...mainly determined by ε_T [54], which ...

134:... (a) Typical...

134:...(a)Typical hysteresis loop of ferroelectric materials.(b) Defifinition ...

136:... Communications.(c) dIllustration...

139:...ε_T and ...

158:...poly-crystalline materials, the highly ...

162:...and electroscopes and strong magnetic...

163:...and Rolling-assisted Biaxially Textured Substrates [68]....

169:... Ref.[32]Copyright 2020，Info-mat....

170:... International.(c) Reactive...

172:...evolution of Pb(Zr_xTi_1-x)O₃ micro...

173:...from Ref.[42] Copyright 2023,...

173:... International.(e) SEM ...

175:... Solids.(f) SEM micro...

176:...from Ref.[48] Copyright ...

180:...[71] Copyright 2015.Journal of Materials Research. (i) Schematic...

184:...Ref.[33] Copyright ...

186:...Ref.[35] Copyright ...

257:...Fig. 4(c), Li et al. [80] applied...

266:...Figure 4. (a) Hot-press ...

267:...2023,Elsevier.(b) SEM ...

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327:_...(a) Schematic illustration ...

329:...(b) EBSD micrographs of...

331:... ACS. (c) Unipolar ...

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379:...the F₀₀₁ of the...

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386:...ACS. (c) Dielectric...

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470:... replace (Bi_0.5Na_0.5) ²⁺ MPC...

472:...between (Bi_0.5Na_0.5)²⁺ ...

505:...solid-state method. Higher piezoelectricity was subsequently achieved by constructing ternary ceramics in KNN-based (1-x-y) K_1-wNa_wNb_1-zSb_zO₃-yBaZrO₃-xBi_0.5K_0.5HfO₃ (KNNS-BZ-BKH) ...

574:...Figure 10. (a) Schematic diagram...

575:...Ceramics. (b) ...

582:...(d) Schematic illustration...

585:...ACS. (f) The ...

591:... conventional solid-state reaction (CSSR) method to prepare by RTGG method the woven 0.94Bi_1/2Na_1/2TiO₃-0.06BaZrO₃(BNT-BZ) ceramics,...

595:...(90o-αR = 0.031o) ...

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641:... International.(c) Room temperature...

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691:...d₃₃ (pC/N)...

Reviewer 2 Report

Comments and Suggestions for Authors

When we examine the title, the article seems to be a summary of piezoelectric ceramics, but the content of the article seems to focus on the texture properties of ceramics. It is necessary to emphasize the aspect from which ceramics are discussed in the title. (Such as the effect of ceramic preparation methods on texture, or the effect of texture on electrical properties, etc.)

The preparation method of piezoelectric ceramics is mentioned in the abstract section, there are many piezoelectric ceramics. which class of ceramics focus?

In the sentence "With the rapid advancement of science and technology and the rapid development of artificial intelligence technology, the research and development of smart materials is of key importance", what is the connection between the rapid development of science and technology and artificial intelligence technology and the need for smart materials? Why different ceramics? It needs to be detailed.

In the introduction, it is stated that In this article, we will introduce in detail the process flow of the texturing technique and the development of the application of the texturing process in the field of high-performance piezoelectric ceramics in recent years. In the abstract, this article first introduces the performance parameters of piezoelectric ceramics, then summarizes the effect of various preparation processes on the performance of piezoelectric ceramics, and finally summarizes the parameters of high-tech ceramics reported this year, and looks forward to the future preparation of high-tech ceramic materials. Which? or how should be emphasized or should be stated as the texture role of material preparation

Author Response

Comment 1:

1. the article seems to be a summary of piezoelectric ceramics, but the content of the article seems to focus on the texture properties of ceramics. It is necessary to emphasize the aspect from which ceramics are discussed in the title. (Such as the effect of ceramic preparation methods on texture, or the effect of texture on electrical properties, etc.)

Response:

Thank you for your comments. There is a close relationship between piezoelectric ceramics and texturing processes. Texturing processes primarily optimize the electrical, mechanical, and physical properties of ceramic materials by controlling the orientation of the grains within the material. During the manufacturing of piezoelectric ceramics, the texturing process can significantly enhance the material's piezoelectric effect, electromechanical coupling coefficient, mechanical strength, and thermal stability. The following are some key aspects of the relationship between piezoelectric ceramics and the texturing process:

The piezoelectric effect, electromechanical coupling coefficient , and other properties of piezoelectric ceramics are largely influenced by the arrangement of their grains. Traditional piezoelectric ceramics typically have random grain orientations, which limits their piezoelectric and mechanical properties. Through texturing processes, ceramic particles or crystals can be aligned in a specific direction, which significantly improves their performance. The specific improvements are as follows:

Enhancing Piezoelectric Effect: Textured ceramics can increase the piezoelectric constant (such as

d₃₃ by aligning the grains in a specific direction. This directional alignment strengthens the material's ability to deform mechanically under the influence of an electric field, making it more efficient in converting electrical energy into mechanical energy.

Enhancing Electromechanical Coupling Coefficient: The electromechanical coupling coefficient of piezoelectric ceramics is closely related to the orientation of the ceramic grains. The texturing process optimizes the grain directionality, thus improving the material's electromechanical coupling ability. A high electromechanical coupling coefficient means that piezoelectric ceramics can more effectively convert electrical energy into mechanical energy, enhancing the efficiency of actuators and sensors.

Improving Mechanical Properties: Textured ceramics typically exhibit higher mechanical strength, toughness, and fatigue resistance. This is because the directional arrangement of grains allows the material to better withstand external mechanical stresses, preventing fracture or performance degradation during use.

Improving Thermal Stability: The ordered arrangement of grains helps enhance the material's thermal stability, allowing textured ceramics to maintain better performance in high-temperature environments. Compared to traditional ceramics, textured ceramics demonstrate stronger thermal stability under extreme temperature conditions.

This paper aims to compile the preparation processes of various high-performance piezoelectric ceramics in recent years, primarily focusing on the performance of piezoelectric ceramics as the basis for demonstrating the development and application of these processes. A detailed classification of the most efficient and widely applied texturing processes is provided, and the latest research achievements in the field of piezoelectric ceramics through texturing processes are summarized. Therefore, the title is proposed to be modified to Development Status of Textured Piezoelectric Ceramics and Preparation Processes.

Comment 2:

2. The preparation method of piezoelectric ceramics is mentioned in the abstract section, there are many piezoelectric ceramics. which class of ceramics focus? In the sentence "With the rapid advancement of science and technology and the rapid development of artificial intelligence technology, the research and development of smart materials is of key importance", what is the connection between the rapid development of science and technology and artificial intelligence technology and the need for smart materials? Why different ceramics? It needs to be detailed.

Response:

Thank you for your comments.

The rapid development of science and technology, along with advancements in Artificial Intelligence (AI), has closely driven the increasing demand for piezoelectric materials, especially in the applications of automation, intelligent devices, and high-performance sensors. As these technologies continue to progress, the requirements for piezoelectric materials have become increasingly demanding. Below are several key connections between the growth of demand for piezoelectric materials and advancements in science and AI:

1. Technological Advancements Driving the Demand for High-Performance Piezoelectric Materials

The rapid progress of science and technology, particularly in the following areas, has raised the performance requirements for piezoelectric materials:

Automation and Intelligent Devices: With the continuous development of industrial automation, the Internet of Things (IoT), smart homes, and robotics, the application of piezoelectric materials in sensors, actuators, and transducers has been expanding. These intelligent devices require high-performance piezoelectric materials to achieve high sensitivity, fast response, and stable operation. For instance, piezoelectric sensors in smart homes can monitor environmental changes in real-time and provide feedback control, while intelligent robots require efficient piezoelectric drive systems for precise movement.

Medical Technology and Biomedicine: Piezoelectric materials are widely used in medical devices such as ultrasound imaging, diagnostic equipment, and therapeutic devices. As medical diagnostic technology advances and the demand for higher precision and smaller-sized devices increases, the performance requirements for piezoelectric materials continue to grow. For example, high-resolution ultrasound devices require piezoelectric sensors with high sensitivity, stability, and adaptability.

Energy Harvesting and Environmental Monitoring: With the growing demand for sustainable development and clean energy, the application of piezoelectric materials in energy harvesting (such as vibration energy harvesting) and environmental monitoring (such as sensors) is also increasing. These applications require piezoelectric materials to operate stably in extreme environments and have high energy conversion efficiency.

Miniaturization and High Efficiency: As devices become smaller and more integrated, the performance requirements for materials continue to rise. Piezoelectric materials need to have higher efficiency, smaller size, better stability, and stronger adaptability to meet the needs of compact, high-efficiency devices.

 

2. Artificial Intelligence Driving the Demand for Piezoelectric Materials

The advancement of AI, particularly in data processing, intelligent control, and adaptive systems, has had a profound impact on the demand for piezoelectric materials. The application of AI has led to an increasing demand for piezoelectric materials in the following areas:

Intelligent Sensing and Feedback Systems: AI technology enables sensors to automatically analyze and process environmental data through intelligent algorithms, subsequently adjusting the device's operating state. Piezoelectric sensors, being the core component, require high sensitivity and fast response, while also maintaining stable performance under varying environmental conditions. With AI assistance, the application of piezoelectric materials in sensors becomes more precise and efficient, especially in smart manufacturing, environmental monitoring, and healthcare.

Adaptive and Self-Learning Material Systems: As AI technology continues to evolve, many systems are becoming adaptive and self-learning, meaning piezoelectric materials need to automatically adjust their operating state in response to environmental changes. For example, AI-driven piezoelectric materials can automatically adjust their performance based on data collected by sensors to respond to external changes such as temperature, pressure, or vibration. This adaptability is crucial for many high-precision applications, such as intelligent robots, smart sensors, and wearable devices.

Multifunctional Material Systems: With AI's application across various fields, the multifunctionality and intelligence of materials have become increasingly important. AI enables piezoelectric materials to integrate more functions, such as energy harvesting, sensing, and actuation, all within a single system. For instance, AI can analyze real-time data collected from piezoelectric sensors and determine how to adjust the material's performance to optimize device performance under different operating conditions.

Comment 3:

2. In the introduction, it is stated that In this article, we will introduce in detail the process flow of the texturing technique and the development of the application of the texturing process in the field of high-performance piezoelectric ceramics in recent years. In the abstract, this article first introduces the performance parameters of piezoelectric ceramics, then summarizes the effect of various preparation processes on the performance of piezoelectric ceramics, and finally summarizes the parameters of high-tech ceramics reported this year, and looks forward to the future preparation of high-tech ceramic materials. Which? or how should be emphasized or should be stated as the texture role of material preparation

Response:

Thank you for your comments.

 

This article introduces the processes for preparing high-performance piezoelectric ceramics, with a focus on the performance of piezoelectric ceramics as the main thread. The abstract introduces the key factors that determine their performance—namely, the preparation processes—through the performance of piezoelectric ceramics. The introduction first discusses the current demand for high-performance piezoelectric ceramics, highlighting the necessity of developing high-performance piezoelectric ceramics. It then lists the advantages of both lead-based and lead-free ceramics, and finally introduces the preparation processes for high-performance lead-free ceramics. Therefore, the introduction section has been modified as follows:

 With the increasing demands for the performance of piezoelectric materials, particularly in the fields of electronics, sensors, and medical devices, traditional piezoelectric ceramics often fail to meet the requirements of high-performance materials due to the limitations of grain arrangement[1]. In this context, textured ceramics have emerged as a solution. Textured piezoelectric ceramics refer to ceramics where the grains or crystals are oriented in a specific direction through certain processing techniques, thus achieving superior electromechanical properties[2,3]. Compared to traditional ceramics with random grain arrangements, textured piezoelectric ceramics can significantly improve the material's piezoelectric performance, mechanical strength, and other physical properties[4,5]. The fabrication of textured ceramics not only addresses the performance bottlenecks of traditional materials under high-frequency, high-voltage, and high-temperature conditions but also provides higher efficiency and broader application prospects [6-9].

In the past, lead-based ceramics such as PZT [10-12], PMN-PT[13-15], and PLZT[16-17] were widely used. Common lead-free ceramics, such as BNT-BT[18-21], BKT[22,23], and KNN[24,25], generally cannot match the performance of lead-based ceramics, which is why lead-based ceramics remain the mainstream material for most commercial MLA. However, with the growing environmental awareness, the environmental impact of lead-based ceramics has become increasingly apparent, and the development of lead-free ceramics has become a hot topic in the current research on functional ceramics [26-31].