Cryogenics 119 (2021) 103353 Contents lists available at ScienceDirect Cryogenics journal homepage: www.elsevier.com/locate/cryogenics Structural and superconducting properties of low-density Bi(Pb)-2223 superconductor: Effect of Eu2O3 nanoparticles addition E.S. Nurbaisyatul a, H. Azhan b, *, N. Ibrahim a, S.F. Saipuddin a, b a b Faculty of Applied Sciences, Universiti Teknologi MARA Shah Alam, 40450 Shah Alam, Selangor, Malaysia Faculty of Applied Sciences, Universiti Teknologi MARA Pahang, 26400 Bandar Tun Abdul Razak Jengka, Pahang, Malaysia A R T I C L E I N F O A B S T R A C T Keywords: Bi(Pb)-2223 Rare earth nanoparticles Porous Addition Grain size This paper presented the result of the structural analysis of Europium, Eu nanoparticles addition in low-density Bi (Pb)-2223 superconductor. Polycrystalline bulks with nominal composition Bi1.6Pb0.4Sr2Ca2Cu3Oy + xEu2O3 samples where x = 0.0, 0.2, 0.4, 0.6 and 0.8 wt% were prepared via solid-state reaction method. Low-density samples were created by adding crystalline sucrose into mixed powders and burn at 400 ◦ C for two hours. The samples were characterized using X-Ray Diffraction (XRD) and Scanning Electron Microscopy (SEM) for structural characterization while resistivity measurement was determined by using four-point probe method. Phase analysis by XRD indicated that both Bi-2212 and Bi-2223 phases coexist within the samples having a tetragonal crystal structure. As Eu concentration increases, the amount of Bi-2223 phase slightly decreased which signifies that Eu nanoparticles favour the growth of Bi-2212 phase. It was observed that the highest Tc and Jc values for the addition sample found at x = 0.2 wt%. 1. Introduction Nowadays, researchers have conducted numerous studies to discover the best materials that can maintain superconductivity at room tem­ perature [1,2]. An extensive search for novel superconductors has been performed to find the best materials with higher critical temperature, Tc. Superconducting materials can be classified into three groups which are metal-based system, copper oxides (cuprates) and iron-based super­ conductors [3]. Among those categories, cuprates exhibit admirable characteristics due to their strong magnetic field performance, zero energy losses and current-carrying capacity [4]. BSCCO system is one of the promising materials that attracted researchers’ attention due to their great capability to carry electrical current without any resistance. This system mainly consists of three phases with general formula Bi2Sr2CanCunO2n+4+y where n = 1, 2 and 3 considering the number of CuO2 layers in the sub-unit cell respectively. Notably, Bi-2223 phases more preferable due to the highest critical temperature, Tc (~110 K) compared to Bi-2201 (~20 K) and Bi-2212 (~90 K) [5]. Different method of preparation, structural and superconducting properties has been reported through the experience of past research [6–11]. There are still lacking in terms of this behaviour although numerous attempts have been made to further understand the phenomenon of a superconductor. Besides BSCCO system, there are other classes of oxide hightemperature superconductor materials such as Y-Ba-Cu-O and Tl-based family (Tl-Ba-Ca-Cu-O) that are also promising for practical uses. The YBCO family has unique characteristic that makes them promising for electronic and magnetic applications, such as particle accelerators, electronic motors and power transmission and magnetic levitator de­ vices. Meanwhile, Tl-based family consist of different phases which are Tl-2212, Tl-1223 and Tl-2223 with critical temperature of more than 120 K but have inability in carrying current in wires and tapes due to incompetence in controlling the crystallographic orientation, grain boundaries and microcracking [12]. One of the possible ways to increase Jc value is through a low-density high-temperature superconductor. Low-density samples are also known as porous samples which have an intermediate medium. According to previous research, sucrose has been used as an additive to produce porous surfaces, as it cannot react with the alumina matrix while burning [13]. Study by Wu, I.J. in 2001 discovered that the Jc values of the porous YBCO films were higher by at least fifty percent rather than the free-pores YBCO films even for thick films [14]. One of the bene­ fits of the porous structure is that it enables effective contact to the sample by applying a silver-conductive paint which then immerses into the body of the sample, making a deep contact instead of applying just * Corresponding author. E-mail address: dazhan@uitm.edu.my (H. Azhan). https://doi.org/10.1016/j.cryogenics.2021.103353 Received 21 January 2021; Received in revised form 24 August 2021; Accepted 29 August 2021 Available online 2 September 2021 0011-2275/© 2021 Elsevier Ltd. All rights reserved. E.S. Nurbaisyatul et al. Cryogenics 119 (2021) 103353 on the surface. Over the past few years, much effort has been taken to prepare the high Tc Bi-2223 phase superconductors. Several synthesizing techniques such as the conventional solid state method [15–18], sol–gel method [19,20] and co-precipitation (COP) method [21,22] have been devel­ oped so that superconductors with desired properties can be obtained. Unfortunately, a major problem rises from previous study which turned out to be intergrain weak links leading to a weak critical current density, Jc. Note that the amount of dopant and additive elements need to be controlled to improve the Jc values. However, the type of additive used must be taken into consideration as it either acts as an impurity or destruct the characteristics of the crystal structure [23]. Normally, the preparation of BSCCO system always leads to the coexistence of Bi-2212 and Bi-2223 phases despite many attempts to obtain Bi-2223 single phase. Subsequently, it is of interest to introduce nano-sized rare earth el­ ements into the porous structure of Bi(Pb)-2223 to increase the con­ nectivity between the grains. In recent years, there is an increasing interest among researchers to use nanomaterials to improve the super­ conductivity characteristic of the BSCCO system. Numerous studies have investigated the effect of substitution or addition of nanomaterials into high-temperature superconductors as demonstrated in [17] and [24–29]. The latest study by Loudhaief et al. investigated the impact of Cadmium Sulfide (CdS) nanoparticles on the superconducting properties and flux pinning ability in Bi(Pb)-2223 superconductor [30]. Based on the result obtained, they found that small addition of Cadmium Sulfide (CdS) nanoparticles (≤0.3 wt%) exhibit the higher critical current densities, Jc and produced strong pinning centres in the Bi(Pb)-2223 system compared to CdS-free sample. The effect of TiO2 nanoparticles addition into YBCO superconductor has been recently studied by Han­ nachi et al. which revealed that adding 0.1 wt% of TiO2 nanoparticles allowed a significant improvement in the connectivity between YBCO grains [23]. Hence, this paper aims to study the influence of the nano­ sized Eu2O3 addition in porous BSCCO compound on the structural and superconducting properties synthesized by solid-state reaction method. In this research, we added Eu2O3 nanoparticles to the BSCCO system to improve the connectivity between the grains owing to the metallic behaviour of Europium. Different parameters such as lattice parameters, hole concentrations, critical temperature (Tc) and critical current den­ sity (Jc) were evaluated and compared. Fig. 1. Crystal structure of Bi-2223 compound according to the results of VESTA software. SrCaCuO superconductor. The low-density pellets were crushed into powder and Eu2O3 nanopowder were added according to different wt% (x = 0.0, 0.2, 0.4, 0.6 and 0.8 wt%) and ground again for one hour. Under the same amount of pressure, the powders were pressed and then sintered at 850 ◦ C for 48 h. Analysis of the structure and phase formation was performed at room temperature using X’Pert PRO PANalytical X-ray Diffractometer (XRD) in a 2θ range of 5◦ to 90◦ . Meanwhile, the fractured pellet was examined using Scanning Electron Microscopy (SEM) and Energy Dispersive X-ray (EDX) to investigate the morphology and elemental composition of the sample. The electrical resistance was measured with a current of 20 mA using the standard four-point probe method over a temperature range of 30 to 300 K controlled using a 12 K closed-cycle He-cryostat system, Lake Shore 9700 Temperature Controller, Keithley 2410 SMU pro­ grammable current source and Keithley 2182A nanovoltmeter. Four wire probes were attached on top and side of the surface sample using Ag-paste where the outer probes carry current, I across the surface while the two inner probes are the voltages probes which measure the voltage, V in between the outer probes. The temperature was measured from 30 2. Methodology In this research, all samples were prepared by the conventional solidstate reactions method. The required proportions of raw materials are weighed of the total weight of 20 g according to BSCCO stoichiometry which is Bi1.6Pb0.4Sr2Ca2Cu3Oy + xEu2O3 where x = 0.0, 0.2, 0.4, 0.6 and 0.8 wt% by using a sensitive weighing balancing model Setra EL200S (±0.0001 g). The solutions of the samples were prepared by mixing Bi2O3, PbO, SrCO3, CaCO3 and CuO powders according to sto­ chiometric weights with an absolute ethanol (99.5% purity) in milling jar together with milling balls. The solutions were wet-milled for 24 h to obtain a well-mixed dark grey slurry. The slurry obtained was dried out in the oven for six hours at 120 ◦ C. Once it was dried, the grey powder was scraped off from the beaker and ground for 30 min in a mortar. There were two calcination processes involved in the making of Bi-2223 sample, both were done in an ambient atmosphere with intermediate grinding. The grey precursor obtained was placed in an alumina boat and undergoes pre-calcination process at 800 ◦ C for 15 h. The second calcination process also subjected to 830 ◦ C for 15 h. The powder was then weighed into 2 g samples and each were pressed under a pressure of 30 Mpa. For porous samples, the powder was weighed together with polycrystalline sucrose, C12H22O11 (weight ratio of mixed powder to sucrose is 1.9500 ± 0.0001 g : 0.0500 ± 0.0001 g). The bulk obtained were heated at 200 ◦ C for two hours to eliminate the sucrose. The porous pellets were sintered at 850 ◦ C for 48 h to produce a single-phase Bi(Pb) Fig. 2. X-ray diffraction patterns of samples with different addition of Eu nanoparticles. 2 E.S. Nurbaisyatul et al. Cryogenics 119 (2021) 103353 Table 1 Lattice parameter and relative volume fraction of different concentration of Eu2O3 nanoparticles addition on low density Bi-2223 superconductor. Samples, x (wt%) 0.0 0.2 0.4 0.6 0.8 Volume [Å 3] Lattice parameter [Å] a b c 5.394 5.406 5.409 5.404 5.409 5.399 5.405 5.403 5.401 5.405 37.149 37.169 37.214 37.041 37.062 1082.1 1086.3 1087.7 1081.2 1083.6 Volume fraction [%] Williamson-Hall Bi-2223 Bi-2212 Crystallite size (nm) Lattice strain, Cε (x10-3) 88.3 83.1 82.0 70.6 71.1 11.7 16.9 18.0 29.4 28.9 32.50 47.10 43.37 42.60 43.66 2.2 4.3 3.2 2.5 3.3 Fig. 3. Volume fraction of Bi-2212 and Bi-2223 phases for different concen­ tration of Eu nanoparticles addition. to 300 K where the critical temperature, Tc zero was defined as the temperature where the resistance starts to diverge from the lowtemperature horizontal line. The XRD peaks intensities that was observed can be used to calculate the relative volume fractions by using the following relations: Bi − 2223 = ΣI(2223) × 100% ΣI(2223) + ΣI(2212) (1) Bi − 2212 = ΣI(2212) × 100% ΣI(2223) + ΣI(2212) (2) Fig. 4. Williamson-Hall (W-H) plots of Bcosθ versus 4sinθ for low density Bi1.6Pb0.4Sr2Ca2Cu3Oy + xEu2O3 where x = 0.0, 0.2, 0.4, 0.6 and 0.8 wt%. along with their relative amounts of Bi-2212 and Bi-2223 phases. Using the least square method, the lattice parameters are calculated through the distances between atomic layers in a crystal, d and (hkl) planes for a tetragonal unit cell structure. Meanwhile, the volume fraction of Bi2212 and Bi-2223 phases for different concentration of Eu nano­ particles addition was calculated using Eqs. (1) and (2) and depicted in Fig. 3. Table 1 indicates that both Bi-2212 and Bi-2223 phases were affaected by the addition of Eu nanoparticles, indicating a reduction in the volume fraction of the Bi-2223 phase. As can be seen, Bi-2223 peaks were most prominent in the Eu-free sample. Previous study by Mahtali, M. and Chamekh, S. mentioned that annealing below 875 ◦ C led to the formation of the secondary phase with single and multilayer Bi com­ pounds [31]. Besides, the effect of Eu substitution on Ca site in Bi(Pb)2223 superconductor prepared via co-precipitation method have been studied, indicating that Eu-doped sample which is sintered at 850 ◦ C for 48 h produce more Bi-2212 phase as Eu concentration increases [9]. Based on the calculated lattice parameter, all sample exhibit a tetragonal structure with different values of lattice parameters. The variation of a and c values for Eu-free and Eu-addition samples has slightly different as Eu addition increases but the crystal structure re­ mains unchanged. This result shows that Eu particles did not engage in the host system. It is consistent with previous research where the crystal where I(2223) and I(2212) refer to the intensities of the Bi-2223 and Bi2212 peak, respectively. 3. Result and discussions Fig. 1 shows the crystal structure of Bi-2223 high-temperature su­ perconductor as presented using the VESTA software. X-ray diffraction patterns for all samples sintered at 850 ◦ C for 48 h were plotted as shown in Fig. 2. The formation of Bi-2212 and Bi-2223 phases were determined through peak matching using Xpert Highscore software. Based on Fig. 2, the Eu-free sample showed a few peaks of low intensity which belongs to Bi-2212 phase and major peaks belonging to the Bi-2223 phase. Mean­ while, the consistency of peaks can be seen for x = 0.2, 0.4, 0.6 and 0.8 wt% samples as the mixed phases of Bi-2212 and Bi-2223 were detected. The peaks for the phases of Bi-2212 and Bi-2223 was indicated by (•) and (*), respectively. XRD patterns clearly demonstrate that the in­ tensity of Bi-2223 phase increased compared to the Eu-free sample apparent at peaks (0111), (2012), (2 2 2) at 2θ = 31.02◦ , 44.65◦ and 47.66◦ respectively. The peak of Bi-2212 phase around 2θ = 24.89◦ and 33.64◦ corresponding to (1 1 3) and (0 2 2) respectively increased as Eu nanoparticles concentration increased. The lattice parameters of the prepared sample are shown in Table 1, 3 E.S. Nurbaisyatul et al. Cryogenics 119 (2021) 103353 Fig. 5. SEM surface micrographs of low-density Bi1.6Pb0.4Sr2Ca2Cu3Oy + xEu2O3 samples (a) x = 0.0, (b) x = 0.2, (c) x = 0.4, (d) x = 0.6 and (e) × = 0.8 wt%. structure of Bi-2223 system remains unchanged when adding with Eu nanoparticles [9]. Furthermore, the decreases in lattice parameters are possibly due to the change in oxygen contents related to the substitution of Eu3+ with higher valence cations [32,33]. It is a very challenging task to understand the effect of substitution on parameters a and b, since these parameters are controlled by the length of the Cu-O bond in the plane [34]. The crystallite size, D of the sample was estimated by applying 4 E.S. Nurbaisyatul et al. Cryogenics 119 (2021) 103353 Fig. 6. Elemental mapping for Bi-2223 sample adding with 0.2 wt% Eu nanoparticles. Scherer equations [35]: D = kλ Bcosθ thus preventing grain growth. Hence, it is noticeable to conclude that the reduce in grain size degrade the connectivity between the super­ conducting grains [38]. Alaghbari et al. reported that when grain size decreases, the weak link increases and ultimately the current can no longer flow between the grains, resulting in a lower Jc [39]. Meanwhile, Kir et al. concludes that some randomly distributed large grains reflect the presence of Bi-2212 phase thus lower the Tc values due to the weak connectivity between grains [33]. Fig. 6 presents the elemental mapping of Bi-2223 adding with x = 0.2 wt% of Eu indicating that this Bi-2223 addition superconductor grains consist of Bi, Pb, Sr, Ca, Cu, O and Eu elements. The summary of composition elements of low-density Bi-2223 added with Er2O3 nano­ particles are tabulated in Table 2. All the elements such as Bismuth, Lead, Strontium, Calcium, Copper and Europium which have been taken initially are present in the atomic% with their appropriate amount. From the results obtained, all the elements are present in the prepared sam­ ples. The presence of Europium nanoparticles in the superconductor system is confirmed with the increment of the composition of Neo­ dymium from 0 up to 0.26 atomic%, respectively. These results defi­ nitely indicate that the Europium nanoparticles have been successfully incorporated into the structure of the low-density Bi-2223. Fig. 7 displays the electrical resistivity versus temperature from 30 K to 300 K for all the samples. As can be seen, a smooth resistivity curve is shown for all samples that correspond to Bi-2223 phase one-step tran­ sition. High-temperature superconductors normally exhibit metallic behaviour in their resistivity up to their onset temperatures, suggesting that the resistance behaviour in this range is determined by the degree of electron–phonon interaction [33]. It is known that the Tc onset values represent the points at which the relationship deviates from the linear trend, while the Tc offset values is considered the point where the elec­ trical resistance approaches zero [40]. The critical onset temperature, Tc onset of the samples were 110, 105, 97, 106 and 107 K for x = 0.0, 0.2, 0.4, 0.6 and 0.8 wt% of Eu nanoparticles addition respectively. The resistivity values corresponding to the Tc onset of the samples are 0.385, 0.550, 0.542, 0.621 and 0.636 Ω cm respectively. From Fig. 7, it is obvious that the sample with x = 0.8 wt% has the highest Tc onset value implying the presence of the many high-sized Bi-2212 grains as stated in XRD analysis. Finding by Kir et al concludes that lower Tc offset values indicate that there might be a large amount of porosity due to the randomly oriented larger grains [33]. Table 3 summarizes the data of Tc onset and Tc offset derived from the resistance versus temperature, R(T) graph. The highest value of Tc offset can be seen at 99 K for the Eu-free sample and 89 K was measured in the sample adding with 0.2 wt% of Eu nanoparticles. However, no conclu­ sion can be drawn as to whether intergrain connectivity has improved or (3) where B is the FWHM of the X-ray peaks, k is a shape factor without dimension with the value of 0.9, θ is the Bragg angle and λ is the wavelength of X-ray (1.5406 Å). Whereas, Williamson-Hall (W-H) the­ ory has been used to calculate the lattice strain, Cε for each sample through equations [36]: Bcosθ = 4Cε sinθ + kλ D (4) It is possible to determine the value of Cε by plotting the graph Bcosθ versus 4sinθ as shown in Fig. 4. The value of Cε was deduced based on the slope of linear fitting of the scattered graph. All the obtained D and Cε values are recorded in Table 1. The crystallite size is slightly increased for sample with 0.2 wt% compared to the Eu-free sample, suggesting that Eu2O3 nanoparticles stimulated crystal growth by filling up the voids within the grain boundary networks in Bi-2223. The development of lattice strain results from the displacement of the atoms with respect to their reference positions in the lattice. Clearly, there is no significant variation found in the lattice strain as the Eu2O3 nanoparticles increases. The highest Cε value was found at 0.2 wt% sample. These strains might be resulting from the lattice shrinkage observed in the lattice parameters calculation [37]. Fig. 5 displays the SEM micrograph of the fractured bulk samples for Eu-free sample and Eu-added samples at a magnification of 10000 X with an energy range of 5.00 kV to 10.00 kV. It is observed that the microstructure of Bi-2223 superconductor exhibit a common flaky layers of plate-like grains. The SEM images of Eu-free sample shows the presence of some pores. These pores lead to poor grains connectivity thus lead to lower Jc values. Furthermore, orientation and grains con­ nectivity for x = 0.8 wt% sample are slightly worsened as the size of flaky layers start to reduce and form smaller plate-like grains and distributed randomly without specific alignment. In addition, calcula­ tion of grain size was extracted from this research using Image J soft­ ware by measuring the average length of both sides of the grain. Noted also the image of Fig. 5 taken at different spot of fractured samples thus yielded different value of grain size. The findings display that the maximum grain size for Eu2O3 nanoparticles addition sample is observed at 0.2 wt%. However, the value of grain size decrease compared to Eu-free sample might be due to the increasing of grain boundaries. As grain growth has always been caused by grain boundary energy, it makes sense that when Eu2O3 nanoparticles were added into Bi-2223 system, they settle within the pores and the edges of the grains 5 E.S. Nurbaisyatul et al. Cryogenics 119 (2021) 103353 Fig. 6. (continued). destructed in Tc offset values for 0.6 wt% and 0.8 wt% samples [41]. The difference between Tc onset and Tc offset is known as transition width difference, ΔTc = Tc onset - Tc offset. From the result obtained, ΔTc occurred for the sample x = 0.6 wt% due to the phase inhomogeneities between grains boundaries [42] and the presence of impurities within the structure of the samples. Meanwhile, the increment in the transition 6 E.S. Nurbaisyatul et al. Cryogenics 119 (2021) 103353 Fig. 6. (continued). width difference, ΔTc values as wt% of Eu nanoparticles increase indi­ cating that more than one phase is present and the weak links between superconducting grains is enhanced [9]. The theoretical density of the pure BSCCO system is about 6.302 g/ cm3 [38]. We determined the densities of samples according to the Archimedes principle by weighing in distilled water and air. The calculated densities are listed in Table 3. The table clearly shows that the density values obtained for addition samples are higher than that of the Eu-free sample. While the maximum density value is attributed to x = 0.2 wt%, the smallest density value belongs to the x = 0.4 wt% for the addition sample. The density values obtained are in the range of 78 to 85% compared to the theoretical values. The variations of the hole-carrier concentration versus Eu content is Table 2 Summary of composition elements in low density Bi-2223 superconductor added with different composition of Eu2O3 nanoparticles. Sample, x (wt%) 0.0 0.2 0.4 0.6 0.8 Element (atomic %) Bi Pb Sr Ca Cu O Eu 11.27 8.61 8.86 8.31 8.76 2.60 1.82 2.83 2.26 2.22 10.22 9.42 9.37 9.02 9.81 13.09 8.94 9.47 9.83 9.27 33.08 16.51 15.42 13.45 16.67 29.74 54.62 53.93 56.95 53.01 0.00 0.08 0.12 0.18 0.26 Fig. 7. Normalized resistance at room temperature for low density Bi1.6Pb0.4Sr2Ca2Cu3Oy + xEu2O3 where x = 0.0, 0.2, 0.4, 0.6 and 0.8 wt%. Fig. 8. Superconductivity transition temperature versus hole concentration. Table 3 The critical temperatures Tc,onset, Tc,zero, ΔTc and hole concentration of low density Bi1.6Pb0.4Sr2Ca2Cu3Oy + xEu2O3 samples (x = 0.0, 0.2, 0.4, 0.6 and 0.8 wt%). Samples, x (wt%) 0.0 0.2 0.4 0.6 0.8 Tc onset 110 105 97 106 107 (K) Tc 99 89 74 59 62 zero (K) ΔTC (K) Hole concentration, p Grain size (µm) Density, ρ (±0.01 g/cm3) Porosity, P (%) 11 15 23 47 45 0.125 0.111 0.097 0.085 0.087 3.678 1.746 1.634 1.552 1.539 4.88 5.38 4.92 5.04 5.25 22.56 14.63 21.93 20.03 16.69 7 E.S. Nurbaisyatul et al. Cryogenics 119 (2021) 103353 nanoparticles into BSCCO system enhance the Jc values due to the improvement of the grains connectivity within Eu nanoparticles addi­ tion. Research by Zelati et al. also pointed out the addition of 0.5 wt% of Dy2O3 nanoparticles into Bi-2223 superconductor increases the Jc values where nanoparticles settle between the grains thus improve the grains connectivity [46]. The latest study by Fallah-Arani et al. revealed that the optimum Jc value for Bi-2223 superconductor adding with Titanium Dioxide nanorods (TiO2-NR) found at a sample with 0.2 wt% TiO2-NR content [4]. 4. Conclusion Low-density Bi(Pb)-2223 samples added with different wt% of Eu nanoparticles were prepared by the standard solid-state reaction method. The transition temperature changed with the increase of the wt % of Eu addition. The optimum value of Tc zero for the addition sample was found at sample x = 0.2 wt%. X-ray diffraction analysis showed both Bi-2223 and Bi-2212 phases coexisted in the samples with tetragonal structure. As the concentration of Eu nanoparticles increased, the vol­ ume fraction calculated from the XRD peaks intensities decreased. All the elements in the prepared samples were present in the Bi(Pb)-2223 system and was comfirmed by EDX analysis. Based on resistivity mea­ surements, the highest value of Tc zero and Jc for the Eu-adding sample corresponded at 0.2 wt% sample. Hole concentrations of the samples were determined from the equation showed decrement as Eu concen­ tration increases. Hence, the best sample in this study was found at x = 0.2 wt% of Eu nanoparticles as it gives the best critical current density values compared to the Eu-free sample. Fig. 9. Variation of critical current density versus temperature. Table 4 Variation of critical current density, Jc at different temperature of Bi1.6Pb0.4Sr2Ca2Cu3Oy + xEu2O3 samples (x = 0.0 , 0.2, 0.4, 0.6 and 0.8 wt%). Samples, x (wt%) 0.0 0.2 0.4 0.6 0.8 Critical current density, JC [A/cm2] 30 K 40 K 50 K 60 K 70 K 0.75 7.29 3.18 3.10 2.40 0.46 6.82 3.07 2.41 2.03 0.34 6.20 2.61 1.10 1.01 0.23 5.27 2.16 0.09 – 0.11 4.19 1.36 – – Declaration of Competing Interest depicted in Fig. 8. The hole concentrations shows parabolic relationship dependence on the critical temperature, Tc. The hole concentrations were determined based on the equations given below: Tc /Tc max = 1 − − 82.6 × (p − − 0.16)2 The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. (5) Acknowledgements where p indicates hole concentrations and Tc max for Bi-2223 samples are considered as 110 K. Previous calculations for the Eu-free Bi-2223 samples had shown that the value of p ranged from 0.116 up to 0.160 [43,44]. Study by Tallon et al. revealed that at p = 0.19 value is where the superconductivity is most sturdy [45]. Despite the fact that this research shows a parabolic relationship, the hole concentration values decrease from 0.125 to 0.087 as Eu addition increases. As suggested by Presland et al., the holes transferred from the Bi2O2 bilayer was distributed uniformly onto the three superconducting CuO2 layers in Bi2223 phase [43]. Hence, it can be said that the Eu addition reduces the grain connectivity of the samples thus decreases the Tc offset values. The critical current density, Jc of the samples was measured in zero magnetic fields at temperatures ranging from 30 K to 70 K as shown in Fig. 9 while Jc values are given in Table 4. The critical current density, Jc values were calculated using the equation: Jc = Ic A The authors wish to thank the Ministry of Higher Education Malaysia (MOHE) for financial support in carrying out this research through Fundamental Research Grant Scheme (FRGS) no. 600- RMI/FRGS 5/3 (74/2016). 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