KR20200037483A - Lead-free piezoelectric ceramic composition and method for lead-free piezoelectric ceramic - Google Patents
Lead-free piezoelectric ceramic composition and method for lead-free piezoelectric ceramic Download PDFInfo
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Abstract
Description
본 발명은 무연 압전 세라믹 조성물 및 무연 압전 세라믹 제조 방법에 관한 것이다. The present invention relates to a lead-free piezoelectric ceramic composition and a method for manufacturing a lead-free piezoelectric ceramic.
압전 세라믹 재료는 압전 현상을 나타내는 재료로서, LCD 백라이트용 트랜스포머, 초정밀 액츄에이터, 초음파 모터, 센서와 에너지 하베스팅 분야 등 다양한 분야에 응용되고 있어 지난 수십 년간 많은 연구가 진행되어 왔다.Piezoelectric ceramic material is a material exhibiting a piezoelectric phenomenon, and has been applied to various fields such as transformers for LCD backlights, ultra-precision actuators, ultrasonic motors, sensors and energy harvesting, and has been studied for many decades.
현재, 주류를 이루고 있는 압전 세라믹 재료는 PZT(Pb(Zr,Ti)O3)계 재료로서 납을 기본으로 한 페로브스카이트 구조의 강유전체 화합물이다. PZT계 재료는 인체에 치명적인 중독 문제를 야기시키며, 납의 휘발은 환경오염을 유발시키기 때문에 이를 원천적으로 해결하기 위해 환경 친화적인 압전 세라믹 재료의 개발에 대한 관심이 점차 고조되고 있다. Currently, the mainstream piezoelectric ceramic material is a PZT (Pb (Zr, Ti) O 3 ) -based material, which is a lead-based perovskite structured ferroelectric compound. PZT-based materials cause fatal poisoning problems to the human body, and since volatilization of lead causes environmental pollution, interest in the development of environmentally friendly piezoelectric ceramic materials is gradually increasing.
따라서 일반적인 무연 압전 세라믹 재료인 BNT((BiNa)TiO3)계, NKN((NaK)NbO5)계 재료의 압전 특성을 향상시키기 위해 많은 연구가 진행되어 왔다. 그럼에도 불구하고 이들의 압전 특성은 PZT계 압전 세라믹스의 압전 특성과 비교하여 여전히 낮은 값(d33=100∼200pC/N)을 나타낸다.Therefore, many studies have been conducted to improve the piezoelectric properties of BNT ((BiNa) TiO 3 ) -based and NKN ((NaK) NbO 5 ) -based materials, which are general lead-free piezoelectric ceramic materials. Nevertheless, their piezoelectric properties still show low values (d 33 = 100 to 200 pC / N) compared to the piezoelectric properties of PZT-based piezoelectric ceramics.
Liu와 Ren에 의해 새로이 발견된 BCTZ((Ba,Ca)(Ti,Zr)O3)계 무연 압전 세라믹 재료는, 페로브스카이트 구조를 가지며, 비교적 높은 전기 기계 변환 상수(kp)와 압전 전하 상수(d33)를 나타내는 BCTZ계 무연 압전 세라믹스에 관한 연구가 최근 활발히 이루어지고 있다 BCTZ ((Ba, Ca) (Ti, Zr) O 3 ) based lead-free piezoelectric ceramic material newly discovered by Liu and Ren has a perovskite structure, relatively high electromechanical conversion constant (k p ) and piezoelectric Studies on BCTZ-based lead-free piezoelectric ceramics exhibiting a charge constant (d 33 ) have been actively conducted in recent years.
관련 선행문헌으로 특허 문헌인 대한민국 공개특허 제2017-0081979호, 비특허 문헌인 "소결온도 변화에 따른 (Ba0 . 85Ca0 .15)(Ti0 . 9Zr0 . 1)O3 세라믹스의 유전 및 압전 특성, 전기전자재료학회논문지, 제27권 제1호 pp. 22-26, 2014년 1월: 이갑수 등"가 있다.No. 2017-0081979 Patent Document related prior to the Republic of Korea Laid-Open Patent Document No., non-patent document is "in accordance with the sintering temperature (Ba 0. 85 Ca 0 .15 ) of (Ti 0. 9 Zr 0. 1) O 3 ceramics Dielectric and piezoelectric properties, Journal of the Korean Institute of Electrical and Electronic Material Engineers, Vol. 27, No. 1 pp. 22-26, January 2014: Lee Gap-soo, and others.
본 발명은 압전 특성이 개선된, BCTZ계 무연 압전 세라믹 조성물 및 BCTZ계 무연 압전 세라믹의 제조 방법을 제공하기 위한 것이다.The present invention is to provide a BCTZ-based lead-free piezoelectric ceramic composition having improved piezoelectric properties and a method for manufacturing a BCTZ-based lead-free piezoelectric ceramic.
상기한 목적을 달성하기 위한 본 발명의 일 실시예에 따르면, BCTZ계 모재료 및 산화구리(CuO)를 포함하며, 상기 무연 압전 세라믹 조성물에서, 상기 산화구리의 중량비는 0.2 wt% 내지 0.4 wt%인 무연 압전 세라믹 조성물을 제공한다.According to an embodiment of the present invention for achieving the above object, including a BCTZ-based base material and copper oxide (CuO), in the lead-free piezoelectric ceramic composition, the weight ratio of the copper oxide is 0.2 wt% to 0.4 wt% A phosphorous lead-free piezoelectric ceramic composition is provided.
또한 상기한 목적을 달성하기 위한 본 발명의 다른 실시예에 따르면, BCTZ계 모재료에 산화 구리가 첨가된 혼합물을 제조하는 단계; 및 1300도(℃) 내지 1450도(℃)의 온도에서 상기 혼합물을 소결하는 단계를 포함하며, 상기 혼합물에서 상기 산화 구리의 중량비는 중량비는 0.2 wt% 내지 0.4 wt%인 무연 압전 세라믹의 제조 방법을 제공한다.In addition, according to another embodiment of the present invention for achieving the above object, preparing a mixture of copper oxide is added to the BCTZ-based parent material; And sintering the mixture at a temperature of 1300 degrees C. to 1450 degrees C., wherein the weight ratio of the copper oxide in the mixture is 0.2 wt% to 0.4 wt%. Gives
본 발명에 따르면, BCTZ계 무연 압전 세라믹 조성물의 압전 특성이 개선될 수 있다. According to the present invention, the piezoelectric properties of the BCTZ-based lead-free piezoelectric ceramic composition can be improved.
도 1은 소결 온도에 따른 무연 압전 세라믹의 전계방출형 주사전자현미경(FE-SEM) 이미지를 나타내는 도면이다.
도 2는 소결 온도에 따른 무연 압전 세라믹의 XRD 그래프를 나타내는 도면이다.
도 3은 소결 온도에 따른 무연 압전 세라믹의 출력 파워를 나타내는 도면이다.1 is a view showing a field emission type scanning electron microscope (FE-SEM) image of a lead-free piezoelectric ceramic according to the sintering temperature.
2 is a view showing an XRD graph of a lead-free piezoelectric ceramic according to the sintering temperature.
3 is a view showing the output power of the lead-free piezoelectric ceramic according to the sintering temperature.
본 발명은 다양한 변경을 가할 수 있고 여러 가지 실시예를 가질 수 있는 바, 특정 실시예들을 도면에 예시하고 상세한 설명에 상세하게 설명하고자 한다. 그러나, 이는 본 발명을 특정한 실시 형태에 대해 한정하려는 것이 아니며, 본 발명의 사상 및 기술 범위에 포함되는 모든 변경, 균등물 내지 대체물을 포함하는 것으로 이해되어야 한다. 각 도면을 설명하면서 유사한 참조부호를 유사한 구성요소에 대해 사용하였다. The present invention can be applied to various changes and may have various embodiments, and specific embodiments will be illustrated in the drawings and described in detail in the detailed description. However, this is not intended to limit the present invention to specific embodiments, and should be understood to include all modifications, equivalents, and substitutes included in the spirit and scope of the present invention. In describing each drawing, similar reference numerals are used for similar components.
이하에서, 본 발명에 따른 실시예들을 상세하게 설명한다.Hereinafter, embodiments according to the present invention will be described in detail.
무연 압전 세라믹 조성물Lead-free piezoelectric ceramic composition
본 발명에 따른 무연 압전 세라믹 조성물은 압전 특성이 개선된 BCTZ계 무연 압전 세라믹 조성물로서, BCTZ계 모재료 및 산화구리(CuO)를 포함한다. The lead-free piezoelectric ceramic composition according to the present invention is a BCTZ-based lead-free piezoelectric ceramic composition having improved piezoelectric properties, and includes a BCTZ-based base material and copper oxide (CuO).
본 발명의 일실시예에 따른 무연 압전 세라믹 조성물에서 산화구리의 중량비는 0.2 wt% 내지 0.4 wt% 사이에서 결정될 수 있다.The weight ratio of copper oxide in the lead-free piezoelectric ceramic composition according to an embodiment of the present invention may be determined between 0.2 wt% and 0.4 wt%.
[표 1]은 BCTZ계 모재료로서, (Ba0 . 85Ca0 .15)(Ti0 . 9Zr0 . 1)O3 분말에 산화구리를 첨가하지 않은 무연 압전 세라믹 조성물과, 부재료로서 중량비 0.1 wt% 내지 0.5 wt%의 산화구리가 첨가된 무연 압전 세라믹 조성물에 대한 압전 특성을 나타내는 표이다.[Table 1] BCTZ system as the parent material, (Ba 0. 85 Ca 0 .15) (Ti 0. 9 Zr 0. 1) O 3 is not added to the lead-free copper oxide powder in the piezoelectric ceramic composition and a weight ratio as the sub material Table showing piezoelectric properties for a lead-free piezoelectric ceramic composition to which 0.1 wt% to 0.5 wt% of copper oxide is added.
압전 특성을 나타내는 파라미터로서, 압전 전압 상수(g33), 압전 전하 상수(d33), 전기 기계 변환 상수(kp) 및 품질 계수(Qm)가 있으며, 압전 전압 상수, 압전 전하 상수 및 전기 기계 변환 상수 값이 클수록, 그리고 품질 계수 값이 작을수록 압전 특성이 우수하다. 특히, 압전 전압 상수는 압전 전하 상수에 비례하고, 유전 상수(dielectric constant)에 반비례하는 값으로서, 유전 상수가 작을수록 커진다.As parameters representing piezoelectric properties, there are piezoelectric voltage constant (g 33 ), piezoelectric charge constant (d 33 ), electromechanical conversion constant (k p ) and quality factor (Q m ), piezoelectric voltage constant, piezoelectric charge constant and electricity The larger the mechanical conversion constant value, and the smaller the quality factor value, the better the piezoelectric properties. In particular, the piezoelectric voltage constant is proportional to the piezoelectric charge constant, and is inversely proportional to the dielectric constant. The smaller the dielectric constant, the larger.
[표 1]을 살펴보면, 산화구리가 중량비 0.2 wt%로 BCTZ계 모재료에 첨가된 경우, 압전 전압 상수와 압전 전하 상수를 곱한 값인 압전 변환 상수(d33×g33) 값이 급격히 증가하고 품질 계수 값이 급격히 작아지며, 산화구리가 중량비 0.3 wt%로 첨가된 경우, 압전 변환 상수 값이 최대치를 나타내며 품질 계수 값이 최소치를 나타냄을 알 수 있다. 그리고 산화구리가 중량비 0.5 wt%로 첨가된 경우 압전 변환 상수 값이 급격히 감소함을 알 수 있다.Looking at [Table 1], when copper oxide is added to the BCTZ-based parent material at a weight ratio of 0.2 wt%, the value of the piezoelectric conversion constant (d33 × g33) multiplied by the piezoelectric voltage constant and the piezoelectric charge constant increases rapidly and the quality factor value It can be seen that when it is rapidly reduced and copper oxide is added at a weight ratio of 0.3 wt%, the piezoelectric conversion constant value represents the maximum value and the quality factor value represents the minimum value. And it can be seen that when the copper oxide is added in a weight ratio of 0.5 wt%, the piezoelectric conversion constant value rapidly decreases.
즉, BCTZ계 모재료에 산화구리가 중량비 0.2 wt% 내지 0.4 wt%로 첨가된 경우 우수한 압전 특성이 나타나며, 특히 산화구리가 중량비 0.3 wt%로 첨가된 경우 가장 좋은 압전 특성이 나타남을 알 수 있다.That is, when copper oxide is added at a weight ratio of 0.2 wt% to 0.4 wt% to the BCTZ-based parent material, excellent piezoelectric properties are exhibited. In particular, when copper oxide is added at a weight ratio of 0.3 wt%, the best piezoelectric properties are exhibited. .
무연 압전 세라믹 제조 방법Lead-free piezoelectric ceramic manufacturing method
도 1 내지 3은 본 발명의 일실시예에 따른 무연 압전 세라믹의 제조 방법을 설명하기 위한 도면으로서, 도 1은 소결 온도에 따른 무연 압전 세라믹의 전계방출형 주사전자현미경(FE-SEM) 이미지를 나타내는 도면이며, 도 2는 소결 온도에 따른 무연 압전 세라믹의 XRD 그래프를 나타내는 도면이다. 그리고 도 3은 소결 온도에 따른 무연 압전 세라믹의 출력 파워를 나타내는 도면이다.1 to 3 is a view for explaining a method of manufacturing a lead-free piezoelectric ceramic according to an embodiment of the present invention, Figure 1 is a field emission type scanning electron microscope (FE-SEM) image of the lead-free piezoelectric ceramic according to the sintering temperature 2 is a diagram showing an XRD graph of a lead-free piezoelectric ceramic according to the sintering temperature. And Figure 3 is a view showing the output power of the lead-free piezoelectric ceramic according to the sintering temperature.
본 발명에 따른 무연 압전 세라믹 제조 방법은, BCTZ계 모재료에 산화 구리가 첨가된 혼합물을 제조하는 단계 및 1300도(℃) 내지 1450도(℃)의 온도에서 혼합물을 소결하는 단계를 포함한다.The method for manufacturing a lead-free piezoelectric ceramic according to the present invention includes a step of preparing a mixture in which copper oxide is added to a BCTZ-based base material and sintering the mixture at a temperature of 1300 ° C (1300 ° C) to 1450 ° C (° C).
일실시예로서, BCTZ계 모재료로 (Ba0 . 85Ca0 .15)(Ti0 . 9Zr0 . 1)O3가 이용되며, 혼합물에서 산화구리의 중량비가 0.2 wt% 내지 0.4 wt%가 되도록 산화구리가 첨가된 혼합물이 제조될 수 있다. 그리고 BaCO3(바륨 카보네이트) 및 CaCO3(칼슘 카보네이트)를 몰비 0.85:0.15, TiO2(이산화 타이타늄) 및 ZrO2(지르코늄 다이옥사이드)를 몰비 0.9:0.1 비율로 혼합 및 분쇄하여 (Ba0 . 85Ca0 .15)(Ti0 . 9Zr0 . 1)O3를 마련할 수 있다.In one embodiment, BCTZ system to the parent material (Ba 0. 85 Ca 0 .15 ) (Ti 0. 9 Zr 0. 1) O 3 is used is a mixture in which the weight ratio of copper oxide 0.2 wt% to 0.4 wt% in A mixture to which copper oxide is added may be prepared. And BaCO 3 (barium carbonate) and CaCO 3 (calcium carbonate) in a molar ratio of 0.85: 0.15, TiO 2 (titanium dioxide) and ZrO 2 (zirconium dioxide), a molar ratio of 0.9: mixed and pulverized to 0.1 ratio (Ba 0 85 Ca. 0 .15) (Ti 0. 9 Zr 0. it is possible to provide a 1) O 3.
도 1 내지 도 3 및 [표 2]는 일실시예로서 산화구리가 중량비 0.3 wt%로 첨가되어 4시간 동안 소결된 무연 압전 세라믹의 압전 특성 데이터를 나타낸다. 소결은, 1300도 ~ 1450도 범위에서 50도씩 온도를 조절하여 이루어졌다. 1 to 3 and Table 2 show piezoelectric property data of a lead-free piezoelectric ceramic sintered for 4 hours by adding copper oxide at a weight ratio of 0.3 wt% as an example. Sintering was performed by controlling the temperature by 50 degrees in the range of 1300 degrees to 1450 degrees.
1300도 미만에서는 소결이 이루어지지 않았으며, 1500도에서는 도 1에 도시된 바와 같이, 무연 압전 세라믹의 표면이 녹아 압전 특성을 측정할 수 없었다. 반면, 1300도 내지 1450도 범위에서는 소결이 이루어졌으며, 도 1에 도시된 바와 같이, 5μm에서 40μm까지 다양한 그레인이 관찰되었다. 소결 온도가 1300도에서 1450도로 증가하면서 그레인의 크기도 증가하였다.Sintering was not performed at less than 1300 degrees, and as shown in FIG. 1 at 1500 degrees, the surface of the lead-free piezoelectric ceramic was melted, so that piezoelectric properties could not be measured. On the other hand, sintering was performed in the range of 1300 degrees to 1450 degrees, and various grains were observed from 5 μm to 40 μm, as shown in FIG. 1. As the sintering temperature increased from 1300 degrees to 1450 degrees, the grain size also increased.
도 2를 참조하면, 소결 온도가 1300도에서 1450도로 증가하면서 (110) 피크가 증가하는데, 이는 무연 압전 세라믹의 표면에 형성된 그레인의 크기와 관련이 있다. 또한 소결 온도가 1500도인 경우 (110) 피크가 감소하고, (200) 피크가 증가하는데, 이는 무연 압전 세라믹의 멜팅(melting) 현상과 관련이 있다.Referring to FIG. 2, as the sintering temperature increases from 1300 degrees to 1450 degrees, the (110) peak increases, which is related to the size of the grain formed on the surface of the lead-free piezoelectric ceramic. In addition, when the sintering temperature is 1500 degrees, the (110) peak decreases and the (200) peak increases, which is related to the melting phenomenon of the lead-free piezoelectric ceramic.
[표 2]를 참조하면, 소결 온도가 높아질수록 무연 압전 세라믹의 압전 특성이 개선되며, 1450도에서 소결된 무연 압전 세라믹의 압전 특성이 가장 우수함을 알 수 있다. 그리고 이러한 압전 특성은 도 3에 도시된 무연 압전 세라믹의 출력 파워를 통해서도 확인할 수 있다. Referring to [Table 2], it can be seen that as the sintering temperature increases, the piezoelectric properties of the lead-free piezoelectric ceramic are improved, and the piezoelectric properties of the lead-free piezoelectric ceramic sintered at 1450 degrees are the best. In addition, the piezoelectric characteristics can be confirmed through the output power of the lead-free piezoelectric ceramic shown in FIG. 3.
도 3은 100Ω에서 100kΩ까지 부하 저항을 변화시켜가며 측정한 무연 압전 세라믹의 출력 파워를 나타낸다. 1300도, 1350도, 1400도, 1450도 각각에서 소결된 무연 압전 세라믹의 출력 파워를 나타낸다. 도 3에 도시된 바와 같이, 소결 온도가 높아질수록 출력 파워 역시 높아지며, 1300도에서 소결된 무연 압전 세라믹의 전력 밀도는 최대 52.63 mW/cm3이지만, 1450도에서 소결된 무연 압전 세라믹의 전력 밀도는 최대 107.9 mW/cm3까지 증가한다.Figure 3 shows the output power of the lead-free piezoelectric ceramic measured by changing the load resistance from 100Ω to 100kΩ. It represents the output power of the lead-free piezoelectric ceramic sintered at 1300 degrees, 1350 degrees, 1400 degrees, and 1450 degrees, respectively. 3, as the sintering temperature increases, the output power also increases, and the power density of the lead-free piezoelectric ceramic sintered at 1300 degrees is up to 52.63 mW / cm 3, but the power density of the lead-free piezoelectric ceramic sintered at 1450 degrees It increases up to 107.9 mW / cm 3 .
이는 [표 2]의 결과와 대응되며, 압전 변환 상수 값이 증가할수록 출력 파워 값 역시 증가함을 알 수 있다.This corresponds to the result in [Table 2], and it can be seen that the output power value increases as the piezoelectric conversion constant value increases.
이상과 같이 본 발명에서는 구체적인 구성 요소 등과 같은 특정 사항들과 한정된 실시예 및 도면에 의해 설명되었으나 이는 본 발명의 보다 전반적인 이해를 돕기 위해서 제공된 것일 뿐, 본 발명은 상기의 실시예에 한정되는 것은 아니며, 본 발명이 속하는 분야에서 통상적인 지식을 가진 자라면 이러한 기재로부터 다양한 수정 및 변형이 가능하다. 따라서, 본 발명의 사상은 설명된 실시예에 국한되어 정해져서는 아니되며, 후술하는 특허청구범위뿐 아니라 이 특허청구범위와 균등하거나 등가적 변형이 있는 모든 것들은 본 발명 사상의 범주에 속한다고 할 것이다.As described above, the present invention has been described by specific matters such as specific components and limited embodiments and drawings, but is provided to help a more comprehensive understanding of the present invention, and the present invention is not limited to the above embodiments , Anyone having ordinary knowledge in the field to which the present invention pertains can make various modifications and variations from these descriptions. Accordingly, the spirit of the present invention should not be limited to the described embodiments, and should not be determined, and all claims that are equivalent or equivalent to the scope of the claims as well as the claims to be described later belong to the scope of the spirit of the invention. .
Claims (6)
BCTZ계 모재료 및 산화구리(CuO)를 포함하며,
상기 무연 압전 세라믹 조성물에서, 상기 산화구리의 중량비는 0.2 wt% 내지 0.4 wt%인
무연 압전 세라믹 조성물.
In the lead-free piezoelectric ceramic composition,
Contains BCTZ-based parent material and copper oxide (CuO),
In the lead-free piezoelectric ceramic composition, the weight ratio of the copper oxide is 0.2 wt% to 0.4 wt%
Lead-free piezoelectric ceramic composition.
상기 산화구리의 중량비는
0.3 wt%인
무연 압전 세라믹 조성물.
According to claim 1,
The weight ratio of the copper oxide
0.3 wt% phosphorus
Lead-free piezoelectric ceramic composition.
상기 BCTZ계 모재료는
(Ba0 . 85Ca0 .15)(Ti0 . 9Zr0 . 1)O3인
무연 압전 세라믹 조성물.
According to claim 1,
The BCTZ-based parent material
(Ba 0. 85 Ca 0 .15 ) (Ti 0. 9 Zr 0. 1) O 3 is
Lead-free piezoelectric ceramic composition.
1300도(℃) 내지 1450도(℃)의 온도에서 상기 혼합물을 소결하는 단계를 포함하며,
상기 혼합물에서 상기 산화 구리의 중량비는 중량비는 0.2 wt% 내지 0.4 wt%인
무연 압전 세라믹의 제조 방법.
Preparing a mixture of copper oxide added to the BCTZ-based parent material; And
Sintering the mixture at a temperature of 1300 degrees (℃) to 1450 degrees (℃),
The weight ratio of the copper oxide in the mixture is 0.2 wt% to 0.4 wt%
Method for manufacturing lead-free piezoelectric ceramic.
상기 혼합물을 소결하는 단계는
상기 1450도의 온도에서 상기 혼합물을 소결하는
무연 압전 세라믹의 제조 방법.
The method of claim 4,
Sintering the mixture is
To sinter the mixture at a temperature of 1450 degrees
Method for manufacturing lead-free piezoelectric ceramic.
상기 산화구리의 중량비는
0.3 wt%인
무연 압전 세라믹의 제조 방법.
The method of claim 4,
The weight ratio of the copper oxide
0.3 wt% phosphorus
Method for manufacturing lead-free piezoelectric ceramic.
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| KR20220117025A (en) * | 2021-02-16 | 2022-08-23 | 한양대학교 산학협력단 | Lead-free piezoelectric ceramic composition and method for lead-free piezoelectric ceramic |
| WO2023113306A1 (en) * | 2021-12-13 | 2023-06-22 | 주식회사 해븐 | Core-shell structured lead-free piezoelectric ceramic having excellent piezoelectric and dielectric properties, and method for manufacturing same |
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| CN111499382A (en) * | 2020-04-28 | 2020-08-07 | 天津大学 | High-temperature-stability double-layer energy storage ceramic and preparation method thereof |
| KR20220117025A (en) * | 2021-02-16 | 2022-08-23 | 한양대학교 산학협력단 | Lead-free piezoelectric ceramic composition and method for lead-free piezoelectric ceramic |
| WO2022177262A1 (en) * | 2021-02-16 | 2022-08-25 | 한양대학교 산학협력단 | Lead-free piezoelectric ceramic composition and method for manufacturing lead-free piezoelectric ceramic |
| WO2023113306A1 (en) * | 2021-12-13 | 2023-06-22 | 주식회사 해븐 | Core-shell structured lead-free piezoelectric ceramic having excellent piezoelectric and dielectric properties, and method for manufacturing same |
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