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1.
Nat Commun ; 15(1): 8356, 2024 Sep 27.
Artículo en Inglés | MEDLINE | ID: mdl-39333137

RESUMEN

Ag2Se shows significant potential for near-room-temperature thermoelectric applications, but its performance and device design are still evolving. In this work, we design a novel flexible Ag2Se thin-film-based thermoelectric device with optimized electrode materials and structure, achieving a high output power density of over 65 W m-2 and a normalized power density up to 3.68 µW cm-2 K-2 at a temperature difference of 42 K. By fine-tuning vapor selenization time, we strengthen the (013) orientation and carrier mobility of Ag2Se films, reducing excessive Ag interstitials and achieving a power factor of over 29 µW cm-1 K-2 at 393 K. A protective layer boosts flexibility of the thin film, retaining 90% performance after 1000 bends at 60°. Coupled with p-type Sb2Te3 thin films and rational simulations, the device shows rapid human motion response and precise servo motor control, highlighting the potential of high-performance Ag2Se thin films in advanced applications.

2.
Nanomaterials (Basel) ; 14(17)2024 Aug 30.
Artículo en Inglés | MEDLINE | ID: mdl-39269083

RESUMEN

Cu2Se is an attractive thermoelectric material due to its layered structure, low cost, environmental compatibility, and non-toxicity. These traits make it a promising replacement for conventional thermoelectric materials in large-scale applications. This study focuses on preparing Cu2Se flexible thin films through in situ magnetron sputtering technology while carefully optimizing key preparation parameters, and explores the physical mechanism of thermoelectric property enhancement, especially the power factor. The films are deposited onto flexible polyimide substrates. Experimental findings demonstrate that films grown at a base temperature of 200 °C exhibit favorable performance. Furthermore, annealing heat treatment effectively regulates the Cu element content in the film samples, which reduces carrier concentration and enhances the Seebeck coefficient, ultimately improving the power factor of the materials. Compared to the unannealed samples, the sample annealed at 300 °C exhibited a significant increase in room temperature Seebeck coefficient, rising from 9.13 µVK-1 to 26.73 µVK-1. Concurrently, the power factor improved from 0.33 µWcm-1K-2 to 1.43 µWcm-1K-2.

3.
Small ; 20(32): e2312003, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38644338

RESUMEN

Enhancing the thermoelectric performance of n-type polycrystalline SnSe is essential, addressing challenges posed by elevated thermal conductivity and compromised power factor inherent in its intrinsic p-type characteristics. This investigation utilized solid-state reactions and spark plasma sintering techniques for the synthesis of n-type SnSe. A significant improvement in the figure of merit (ZT) is achieved through strategic reduction in Se concentration and optimization of crystal orientation. The co-doping with Br and Ge further improves the material; Br amplifies carrier concentration, enhancing electrical conductivity, while Ge introduces effective phonon scattering centers. In the Br/Ge co-doped SnSe sample, thermal conductivity dropped to 0.38 Wm⁻¹K⁻¹, yielding a remarkable power factor of 662 µW mK- 2 at 773 K, culminating in a ZT of 1.34. This signifies a noteworthy 605% improvement over the pristine sample, underscoring the pivotal role of Ge doping in enhancing n-type material thermoelectric properties. The enhancement is attributed to Br doping introducing additional electronic states near the valence band, and Ge doping modifying the band structure, fostering resonant states near the conduction band. The Br/Ge co-doping further transforms the band structure, influencing electrical conductivity, Seebeck coefficient, and thermal conductivity, advancing the understanding and application of n-type SnSe materials for superior thermoelectric performance.

4.
Adv Mater ; 36(23): e2313101, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38417448

RESUMEN

Skin-like thermoelectric (TE) films with temperature- and strain-sensing functions are highly desirable for human-machine interaction systems and wearable devices. However, current TE films still face challenges in achieving high flexibility and excellent sensing performance simultaneously. Herein, for the first time, a facile roll-to-roll strategy is proposed to fabricate an ultraflexible chalcogenide glass-polytetrafluoroethylene composite film with superior temperature- and strain-sensing performance. The unique reticular network of the composite film endows it with efficient Seebeck effect and flexibility, leading to a high Seebeck coefficient (731 µV/K), rapid temperature response (≈0.7 s), and excellent strain sensitivity (gauge factor = 836). Based on this high-performance composite film, an intelligent robotic hand for action feedback and temperature alarm is fabricated, demonstrating its great potential in human-machine interaction. Such TE film fabrication strategy not only brings new inspiration for wearable inorganic TE devices, but also sets the stage for a wide implementation of multifunctional human-machine interaction systems.

5.
Nat Commun ; 15(1): 923, 2024 Jan 31.
Artículo en Inglés | MEDLINE | ID: mdl-38296942

RESUMEN

Exploring new near-room-temperature thermoelectric materials is significant for replacing current high-cost Bi2Te3. This study highlights the potential of Ag2Se for wearable thermoelectric electronics, addressing the trade-off between performance and flexibility. A record-high ZT of 1.27 at 363 K is achieved in Ag2Se-based thin films with 3.2 at.% Te doping on Se sites, realized by a new concept of doping-induced orientation engineering. We reveal that Te-doping enhances film uniformity and (00l)-orientation and in turn carrier mobility by reducing the (00l) formation energy, confirmed by solid computational and experimental evidence. The doping simultaneously widens the bandgap, resulting in improved Seebeck coefficients and high power factors, and introduces TeSe point defects to effectively reduce the lattice thermal conductivity. A protective organic-polymer-based composite layer enhances film flexibility, and a rationally designed flexible thermoelectric device achieves an output power density of 1.5 mW cm-2 for wearable power generation under a 20 K temperature difference.

6.
Adv Mater ; 36(5): e2308522, 2024 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-37922408

RESUMEN

Antimony triselenide (Sb2 Se3 ) has possessed excellent optoelectronic properties and has gained interest as a light-harvesting material for photovoltaic technology over the past several years. However, the severe interfacial and bulk recombination obviously contribute to significant carrier transport loss thus leading to the deterioration of power conversion efficiency (PCE). In this work, buried interface and heterojunction engineering are synergistically employed to regulate the film growth kinetic and optimize the band alignment. Through this approach, the orientation of the precursor films is successfully controlled, promoting the preferred orientational growth of the (hk1) of the Sb2 Se3 films. Besides, interfacial trap-assisted nonradiative recombination loss and heterojunction band alignment are successfully minimized and optimized. As a result, the champion device presents a PCE of 9.24% with short-circuit density (JSC ) and fill factor (FF) of 29.47 mA cm-2 and 63.65%, respectively, representing the highest efficiency in sputtered-derived Sb2 Se3 solar cells. This work provides an insightful prescription for fabricating high-quality Sb2 Se3 thin film and enhancing the performance of Sb2 Se3 solar cells.

7.
ACS Appl Mater Interfaces ; 15(51): 59768-59775, 2023 Dec 27.
Artículo en Inglés | MEDLINE | ID: mdl-38085539

RESUMEN

Wearable thermal sensors based on thermoelectric (TE) materials with high sensitivity and temperature resolution are extensively used in medical diagnosis, human-machine interfaces, and advanced artificial intelligence. However, their development is greatly limited by the lack of materials with both a high Seebeck coefficient and superior anticrystallization ability. Here, a new inorganic amorphous TE material, Ge15Ga10Te75, with a high Seebeck coefficient of 1109 µV/K is reported. Owing to the large difference between the glass-transition temperature and initial crystallization temperature, Ge15Ga10Te75 strongly inhibits crystallization during fiber fabrication by thermally codrawing a precast rod comprising a Ge15Ga10Te75 core and PP polymer cladding. The temperature difference can be effectively transduced into electrical signals to achieve TE fiber thermal sensing with an accurate temperature resolution of 0.03 K and a fast response time of 4 s. It is important to note that after the 1.5 and 5.5 K temperatures changed repeatedly, the TE properties of the fiber demonstrated high stability. Based on the Seebeck effect and superior flexibility of the fibers, they can be integrated into a mask and wearable fabric for human respiration and body temperature monitoring. The superior thermal sensing performance of the TE fibers together with their natural flexibility and scalable fabrication endow them with promising applications in health-monitoring and intelligent medical systems.

8.
ACS Appl Mater Interfaces ; 15(40): 47158-47167, 2023 Oct 11.
Artículo en Inglés | MEDLINE | ID: mdl-37782895

RESUMEN

Herein, an n-type Ag2Se thermoelectric flexible thin film has been fabricated on a polyimide (PI) substrate via a novel thermal diffusion method, and the thermoelectric performance is well-optimized by adjusting the pressure and temperature of thermal diffusion. All of the Ag2Se films are beneficial to grow (013) preferred orientations, which is conducive to performing a high Seebeck coefficient. By increasing the thermal diffusion temperature, the electrical conductivity can be rationally regulated while maintaining the independence of the Seebeck coefficient, which is mainly attributed to the increased electric mobility. As a result, the fabricated Ag2Se thin film achieves a high power factor of 18.25 µW cm-1 K-2 at room temperature and a maximum value of 21.7 µW cm-1 K-2 at 393 K. Additionally, the thermal diffusion method has resulted in a wave-shaped buckling, which is further verified as a promising structure to realize a larger temperature difference by the simulation results of finite element analysis (FEA). Additionally, this unique surface morphology of the Ag2Se thin film also exhibits outstanding mechanical properties, for which the elasticity modulus is only 0.42 GPa. Finally, a flexible round-shaped module assembled with Sb2Te3 has demonstrated an output power of 166 nW at a temperature difference of 50 K. This work not only introduces a new method of preparing Ag2Se thin films but also offers a convincing strategy of optimizing the microstructure to enhance low-grade heat utilization efficiency.

9.
Adv Sci (Weinh) ; 10(26): e2302869, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-37391392

RESUMEN

Cadmium sulfide (CdS) buffer layer is commonly used in Kesterite Cu2 ZnSn(S,Se)4 (CZTSSe) thin film solar cells. However, the toxicity of Cadmium (Cd) and perilous waste, which is generated during the deposition process (chemical bath deposition), and the narrow bandgap (≈2.4 eV) of CdS restrict its large-scale future application. Herein, the atomic layer deposition (ALD) method is proposed to deposit zinc-tin-oxide (ZTO) as a buffer layer in Ag-doped CZTSSe solar cells. It is found that the ZTO buffer layer improves the band alignment at the Ag-CZTSSe/ZTO heterojunction interface. The smaller contact potential difference of the ZTO facilitates the extraction of charge carriers and promotes carrier transport. The better p-n junction quality helps to improve the open-circuit voltage (VOC ) and fill factor (FF). Meanwhile, the wider bandgap of ZTO assists to transfer more photons to the CZTSSe absorber, and more photocarriers are generated thus improving short-circuit current density (Jsc). Ultimately, Ag-CZTSSe/ZTO device with 10 nm thick ZTO layer and 5:1 (Zn:Sn) ratio, Sn/(Sn + Zn): 0.28 deliver a superior power conversion efficiency (PCE) of 11.8%. As far as it is known that 11.8% is the highest efficiency among Cd-free kesterite thin film solar cells.

10.
Materials (Basel) ; 16(9)2023 Apr 27.
Artículo en Inglés | MEDLINE | ID: mdl-37176295

RESUMEN

Photoelectrochemical (PEC) water splitting in a pH-neutral electrolyte has attracted more and more attention in the field of sustainable energy. Bismuth vanadate (BiVO4) is a highly promising photoanode material for PEC water splitting. Additionally, cobaltous phosphate (CoPi) is a material that can be synthesized from Earth's rich materials and operates stably in pH-neutral conditions. Herein, we propose a strategy to enhance the charge transport ability and improve PEC performance by electrodepositing the in situ synthesis of a CoPi layer on the BiVO4. With the CoPi co-catalyst, the water oxidation reaction can be accelerated and charge recombination centers are effectively passivated on BiVO4. The BiVO4/CoPi photoanode shows a significantly enhanced photocurrent density (Jph) and applied bias photon-to-current efficiency (ABPE), which are 1.8 and 3.2 times higher than those of a single BiVO4 layer, respectively. Finally, the FTO/BiVO4/CoPi photoanode displays a photocurrent density of 1.39 mA cm-2 at 1.23 VRHE, an onset potential (Von) of 0.30 VRHE, and an ABPE of 0.45%, paving a potential path for future hydrogen evolution by solar-driven water splitting.

11.
Artículo en Inglés | MEDLINE | ID: mdl-36880785

RESUMEN

Kesterite-based Cu2ZnSnS4 (CZTS) thin-film photovoltaics involve a serious interfacial dilemma, leading to severe recombination of carriers and insufficient band alignment at the CZTS/CdS heterojunction. Herein, an interface modification scheme by aluminum doping is introduced for CZTS/CdS via a spin coating method combined with heat treatment. The thermal annealing of the kesterite/CdS junction drives the migration of doped Al from CdS to the absorber, achieving an effective ion substitution and interface passivation. This condition greatly reduces interface recombination and improves device fill factor and current density. The JSC and FF of the champion device increased from 18.01 to 22.33 mA cm-2 and 60.24 to 64.06%, respectively, owing to the optimized band alignment and remarkably enhanced charge carrier generation, separation, and transport. Consequently, a photoelectric conversion efficiency (PCE) of 8.65% was achieved, representing the highest efficiency in CZTS thin-film solar cells fabricated by pulsed laser deposition (PLD) to date. This work proposed a facile strategy for interfacial engineering treatment, opening a valuable avenue to overcome the efficiency bottleneck of CZTS thin-film solar cells.

12.
Materials (Basel) ; 16(3)2023 Feb 02.
Artículo en Inglés | MEDLINE | ID: mdl-36770277

RESUMEN

The Skutterudites CoSb3 material has been the focus of research for the conversion applications of waste heat to electricity due to its ability to accommodate a large variety of ions in the cages that have been proven effective in improving the thermoelectric performance. Although the co-doped CoSb3 bulk materials have attracted increasing attention and have been widely studied, co-doped CoSb3 thin films have been rarely reported. In this work, Ag and Ti were co-doped into CoSb3 thin films via a facile in situ growth method, and the influence of doping content in the thermoelectric properties was investigated. The results show that all the Ag and Ti co-doped CoSb3 thin films contain a pure well-crystallized CoSb3 phase. Compared to the un-doped thin film, the co-doped samples show simultaneous increase in the Seebeck coefficient and the electrical conductivity, leading to a distinctly enhanced power factor. The high power factor value can reach ~0.31 mWm-1K-2 at 623 K after appropriate co-doping, which is two times the value of the un-doped thin film we have been obtained. All the results show that the co-doping is efficient in optimizing the performance of the CoSb3 thin films; the key point is to control the doping element content so as to obtain high thermoelectric properties.

13.
Nanomaterials (Basel) ; 13(2)2023 Jan 07.
Artículo en Inglés | MEDLINE | ID: mdl-36678010

RESUMEN

For thermoelectric thin film, the substrate plays an important role during the growing process and produces effects on its thermoelectric properties. Some special kinds of substrates provide an optimal combination of influences on both the structure and thermoelectric properties. In this work, Bi-Sb-Te films are deposited on Si substrates with different initial orientations by magnetron sputtering in two ways: with and without a pre-coating process. The preferred orientations of the Bi-Sb-Te films are greatly affected by the substrates, in which the thin film tends to deposit on Si substrate with (100) initial orientation and high (015)-texture, while the (00l)-textured Bi-Sb-Te film easily deposits on Si substrate with (110) initial orientation. The experimental and theoretical calculation results indicate that Bi-Sb-Te film with (00l)-texture presents good electrical conductivity and a higher power factor than that of film with (015)-texture.

14.
ACS Appl Mater Interfaces ; 14(28): 31986-31997, 2022 Jul 20.
Artículo en Inglés | MEDLINE | ID: mdl-35793154

RESUMEN

Antimony sulfide-selenide (Sb2(S,Se)3) is a promising light-harvesting material for stable and high-efficiency thin-film photovoltaics (PV) because of its excellent light-harvesting capability, abundant elemental storage, and excellent stability. This study aimed to expand the application of Sb2(S,Se)3 solar cells with a substrate structure as a flexible or tandem device. The use of a hydrothermal method accompanied by a postselenization process for the deposition of Sb2(S,Se)3 film based on the solar cell substrate structure was first demonstrated. The mechanism of postselenization treatment on crystal growth promotion of the Sb2(S,Se)3 film and the defect passivation of the Sb2(S,Se)3 solar cell were revealed through different characterization methods. The crystallinity and the carrier transport property of the Sb2(S,Se)3 film improved, and both the interface defect density of the Sb2(S,Se)3/CdS interface and the bulk defect density of the Sb2(S,Se)3 absorber decreased. Through these above-mentioned processes, the transport and collection of electronics can be improved, and the defect recombination loss can be reduced. By using postselenization treatment to optimize the absorber layer, Sb2(S,Se)3 solar cells with the configuration SLG/Mo/Sb2(S,Se)3/CdS/ITO/Ag achieved an efficiency of 4.05%. This work can provide valuable information for the further development and improvement of Sb2(S,Se)3 solar cells.

15.
Nanomaterials (Basel) ; 12(14)2022 Jul 15.
Artículo en Inglés | MEDLINE | ID: mdl-35889658

RESUMEN

The Te-free compound Bi2SeS2 is considered as a potential thermoelectric material with less environmentally hazardous composition. Herein, the effect of iodine (I) substitution on its thermoelectric transport properties was studied. The electrical conductivity was enhanced due to the increased carrier concentration caused by the carrier provided defect Ise. Thus, an enhanced power factor over 690 µWm−1K−2 was obtained at 300 K by combining a moderate Seebeck coefficient above 150 µV/K due to its large effective mass, which indicated iodine was an effective n-type dopant for Bi2SeS2. Furthermore, a large drop in the lattice thermal conductivity was observed due to the enhanced phonon scattering caused by nanoprecipitates, which resulted in a low total thermal conductivity (<0.95 Wm−1K−1) for all doped samples. Consequently, a maximum ZT value of 0.56 was achieved at 773 K for a Bi2Se1−xIxS2 (x = 1.1%) sample, a nearly threefold improvement compared to the undoped sample.

16.
Adv Mater ; 34(14): e2109078, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35104384

RESUMEN

Despite the fact that antimony triselenide (Sb2 Se3 ) thin-film solar cells have undergone rapid development in recent years, the large open-circuit voltage (VOC ) deficit still remains as the biggest bottleneck, as even the world-record device suffers from a large VOC deficit of 0.59 V. Here, an effective interface engineering approach is reported where the Sb2 Se3 /CdS heterojunction (HTJ) is subjected to a post-annealing treatment using a rapid thermal process. It is found that nonradiative recombination near the Sb2 Se3 /CdS HTJ, including interface recombination and space charge region recombination, is greatly suppressed after the HTJ annealing treatment. Ultimately, a substrate Sb2 Se3 /CdS thin-film solar cell with a competitive power conversion efficiency of 8.64% and a record VOC of 0.52 V is successfully fabricated. The device exhibits a much mitigated VOC deficit of 0.49 V, which is lower than that of any other reported efficient antimony chalcogenide solar cell.

17.
ACS Appl Mater Interfaces ; 14(3): 4276-4284, 2022 Jan 26.
Artículo en Inglés | MEDLINE | ID: mdl-35034451

RESUMEN

Antimony selenosulfide, Sb2(SSe)3, is recognized as an excellent photoactive material owing to its light harvesting capability. There is still room for improvement of the film quality for device performance improvement. Herein, an organic chloride salt [diethylamine hydrochloride, DEA(Cl)] has been introduced for fabricating Sb2(SSe)3 solar cells for the first time. A champion device with a power conversion efficiency (PCE) of 9.17% has been achieved with a relatively improved fill factor and open-circuit voltage (VOC). It has been revealed that DEA(Cl) successfully interacts with Sb2(SSe)3, which can facilitate the crystallization process to give rise to the closely packed bigger grain sizes with reduced surface cracks; it successfully suppressed the oxidized Sb species (Sb2O3) in the Sb2(SSe)3 film to give rise to phase purity, thus leading to superior surface morphology and electrical characteristics of DEA(Cl)-modified Sb2(SSe)3 absorber films. Chloride modification is thus efficiently helpful in suppressing interfacial defects, improving junction quality, and optimizing energy-level alignment. This facile interfacial modification demonstrates the remarkable potential for efficient Sb2(SSe)3 solar cells.

18.
Adv Sci (Weinh) ; 9(9): e2105142, 2022 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-35088583

RESUMEN

Antimony selenide (Sb2 Se3 ) is an ideal photovoltaic candidate profiting from its advantageous material characteristics and superior optoelectronic properties, and has gained considerable development in recent years. However, the further device efficiency breakthrough is largely plagued by severe open-circuit voltage (VOC ) deficit under the existence of multiple defect states and detrimental recombination loss. In this work, an effective absorber layer growth engineering involved with vapor transport deposition and post-selenization is developed to grow Sb2 Se3 thin films. High-quality Sb2 Se3 with large compact crystal grains, benign [hk1] growth orientation, stoichiometric chemical composition, and suitable direct bandgap are successfully fulfilled under an optimized post-selenization scenario. Planar Sb2 Se3 thin-film solar cells with substrate configuration of Mo/Sb2 Se3 /CdS/ITO/Ag are constructed. By contrast, such engineering effort can remarkably mitigate the device VOC deficit, owing to the healed detrimental defects, the suppressed interface and space-charge region recombination, the prolonged carrier lifetime, and the enhanced charge transport. Accordingly, a minimum VOC deficit of 0.647 V contributes to a record VOC of 0.513 V, a champion device with highly interesting efficiency of 7.40% is also comparable to those state-of-the-art Sb2 Se3 solar cells, paving a bright avenue to broaden its scope of photovoltaic applications.

19.
Adv Sci (Weinh) ; 9(5): e2103547, 2022 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-34939357

RESUMEN

Flexible Bi2 Te3 -based thermoelectric devices can function as power generators for powering wearable electronics or chip-sensors for internet-of-things. However, the unsatisfied performance of n-type Bi2 Te3 flexible thin films significantly limits their wide application. In this study, a novel thermal diffusion method is employed to fabricate n-type Te-embedded Bi2 Te3 flexible thin films on flexible polyimide substrates, where Te embeddings can be achieved by tuning the thermal diffusion temperature and correspondingly result in an energy filtering effect at the Bi2 Te3 /Te interfaces. The energy filtering effect can lead to a high Seebeck coefficient ≈160 µV K-1 as well as high carrier mobility of ≈200 cm2 V-1 s-1 at room-temperature. Consequently, an ultrahigh room-temperature power factor of 14.65 µW cm-1 K-2 can be observed in the Te-embedded Bi2 Te3 flexible thin films prepared at the diffusion temperature of 623 K. A thermoelectric sensor is also assembled through integrating the n-type Bi2 Te3 flexible thin films with p-type Sb2 Te3 counterparts, which can fast reflect finger-touch status and demonstrate the applicability of as-prepared Te-embedded Bi2 Te3 flexible thin films. This study indicates that the thermal diffusion method is an effective way to fabricate high-performance and applicable flexible Te-embedded Bi2 Te3 -based thin films.

20.
Nat Commun ; 12(1): 7192, 2021 Dec 10.
Artículo en Inglés | MEDLINE | ID: mdl-34893637

RESUMEN

Nanocomposite engineering decouples the transport of phonons and electrons. This usually involves the in-situ formation or ex-situ addition of nanoparticles to a material matrix with hetero-composition and hetero-structure (heC-heS) interfaces or hetero-composition and homo-structure (heC-hoS) interfaces. Herein, a quasi homo-composition and hetero-structure (hoC-heS) nanocomposite consisting of Pnma Bi2SeS2 - Pnnm Bi2SeS2 is obtained through a Br dopant-induced phase transition, providing a coherent interface between the Pnma matrix and Pnnm second phase due to the slight structural difference between the two phases. This hoC-heS nanocomposite demonstrates a significant reduction in lattice thermal conductivity (~0.40 W m-1 K-1) and an enhanced power factor (7.39 µW cm-1 K-2). Consequently, a record high figure-of-merit ZTmax = 1.12 (at 773 K) and a high average figure-of-merit ZTave = 0.72 (in the range of 323-773 K) are achieved. This work provides a general strategy for synergistically tuning electrical and thermal transport properties by designing hoC-heS nanocomposites through a dopant-induced phase transition.

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