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The organic-inorganic hybrid perovskite solar cells present a rapid improvement on power conversion efficiency from 3.8% to 25.5% in the past decades. Owing to the tuneable bandgaps, low-cost, and ease of fabrication, perovskites become ideal candidate materials for fabricating tandem solar cells, especially for efficient and high-voltage monolithic two-terminal devices. In this review, an overview of recent advances in various monolithic perovskite-based tandem solar cells with a focus on the key challenges is provided. Subsequently, the recombination layer materials, construction of wide-bandgap perovskite layer, stability of narrow-bandgap, and current matching principle in tandems are highlighted in order to optimize the output voltage and conversion efficiency of tandem solar cells. Finally, the recent progress is summarized with a focus on potential applications of tandem solar cells for energy conversion and storage, including hydrogen production by water splitting, CO2 reduction, supercapacitors, and rechargeable batteries, benefiting from the adjustable output voltage of tandem solar cells. It is hoped that this work can offer a feasible strategy to explore more possibilities for fabricating new two-terminal tandem solar cells with high voltage and high conversion efficiency for energy conversion and storage.
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Lithium-sulfur (Li-S) battery is one of the most promising next-generation rechargeable batteries. Lots of fundamental research has been done for the problems during cycling like capacity fading and columbic efficiency reducing owing to severe diffusion and migration of polysulfide intermediates. In the early stage, a wide variety of carbon materials are used as host materials for sulfur to enhance electrical conductivity and adsorb soluble polysulfides. Beyond carbon materials, metal based polar compounds are introduced as host materials for sulfur because of their strong catalytic activity and adsorption ability to suppress the shuttle effect. In addition, relatively high density of metal compounds is helpful for increasing volumetric energy density of Li-S batteries. This review focuses on crystalline multi-metal compounds as host materials in sulfur cathodes. The multi-metal compounds involve not only transition metal composite oxides with specific crystalline structures, binary metal chalcogenides, double or complex salts, but also the metal compounds doped or partially substituted by other metal ions. Generally, for the multi-metal compounds, microstructure and morphologies in micro-nano scale are very significant for mass transfer in electrodes; moreover, adsorption and catalytic ability for polysulfides make fast kinetics in the electrode processes.
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A Li-rich Mn-based layered oxide cathode (LLO) is one of the most promising cathode materials for achieving high-energy lithium-ion batteries. Nevertheless, the intrinsic problems including sluggish kinetics, oxygen evolution, and structural degradation lead to unsatisfactory performance in rate capability, initial Coulombic efficiency, and stability of LLO. Herein, different from the current typical surface modification, an interfacial optimization of primary particles is proposed to improve the simultaneous transport of ions and electrons. The modified interfaces containing AlPO4 and carbon can effectively increase the Li+ diffusion coefficient and decrease the interfacial charge-transfer resistance, thereby achieving fast charge-transport kinetics. Moreover, the in situ high-temperature X-ray diffraction confirms that the modified interface can improve the thermal stability of LLO by inhibiting the lattice oxygen release on the surface of the delithiated cathode material. In addition, the chemical and visual analysis of the cathode-electrolyte interface (CEI) composition clarifies that a highly stable and conductive CEI film generated on the modified electrode can facilitate interfacial kinetic transmission during cycling. As a result, the optimized LLO cathode exhibits a high initial Coulombic efficiency of 87.3% at a 0.2C rate and maintains superior high-rate stability with a capacity retention of 88.2% after 300 cycles at a 5C high rate.
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Simultaneously harvesting, converting and storing solar energy in a single device represents an ideal technological approach for the next generation of power sources. Herein, we propose a device consisting of an integrated carbon-based perovskite solar cell module capable of harvesting solar energy (and converting it into electricity) and a rechargeable aqueous zinc metal cell. The electrochemical energy storage cell utilizes heterostructural Co2P-CoP-NiCoO2 nanometric arrays and zinc metal as the cathode and anode, respectively, and shows a capacity retention of approximately 78% after 25000 cycles at 32 A/g. In particular, the battery cathode and perovskite material of the solar cell are combined in a sandwich joint electrode unit. As a result, the device delivers a specific power of 54 kW/kg and specific energy of 366 Wh/kg at 32 A/g and 2 A/g, respectively. Moreover, benefiting from its narrow voltage range (1.40-1.90 V), the device demonstrates an efficiency of approximately 6%, which is stable for 200 photocharge and discharge cycles.
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Lithium-sulfur batteries with high theoretical energy density have emerged as one of the most promising next-generation rechargeable batteries, while their discharge capacity and cycle stability are challenges mainly due to the shuttle effect of polysulfide intermediates. Employing an effective catalyst for the conversion of polysulfides in cathode reactions can promote the reaction kinetics to restrain the shuttle of polysulfides. Here, for the first time, La2MoO6 (LMO) as a catalyst is introduced into sulfur cathodes. To investigate the effect of La2MoO6, we prepare two different structures of La2MoO6/carbon nanofiber composites. One is carbon nanofiber-supported crystalline La2MoO6 nanoparticles (LMO@CNFs) and the other is amorphous La2MoO6 nanoparticles embedded in carbon nanofibers (LMO-in-CNFs). For sulfur electrodes with â¼73 wt % sulfur loading, LMO@CNFs/S and LMO-in-CNFs/S deliver initial gravimetric capacities of 1493.4 and 1246.7 mA h g-1, respectively, at a 0.1C rate, obviously higher than that of the control sample CNFs/S. Moreover, LMO@CNFs/S shows much better rate performance than LMO-in-CNFs/S, indicating strongly that La2MoO6 is a highly effective catalyst to promote kinetic conversion of polysulfides.
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All-solid-state lithium-sulfur batteries (ASSLSBs) have become a promising candidate because of their high energy density and safety. To ensure the high utilization and electrochemical capacity of sulfur in all-solid-state batteries, both the electronic and ionic conductivities of the sulfur cathode should be as high as possible. In this work, an intercalation-conversion hybrid cathode is proposed by distributing sulfur evenly on electroactive niobium tungsten oxide (Nb18W16O93) and conductive carbon nanotubes (CNTs) for achieving high performance ASSLSBs. Herein, Nb18W16O93 shows good electrochemical lithium storage in the hybrid cathode, which could serve as an effective Li-ion/electron conductor for the conversion of sulfur in the discharge/charge processes to achieve a high utilization of sulfur. However, CNTs could further increase the electronic conductivity of the hybrid cathode by constructing good conductive frameworks and suppress the volumetric fluctuation during the interconversion of sulfur and Li2S. With this strategy, the S/Nb18W16O93/CNT cathode achieves a high sulfur utilization of 91% after one cycle activation with a high gravimetric capacity of 1526 mA h g-1. In addition, excellent rate performance is also obtained at 0.5 C with a reversible capacity of 1262 mA h g-1 after 1000 cycles. This work offers a new perspective to develop ASSLSBs.
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Lithium electrodes have gained increasing attention in recent years for their promising applications in high-energy-density secondary batteries. However, structural instability during cycling remains a considerable obstacle to development. In this study, a dimensionally stable Li-Mg/Cu composite electrode was fabricated. Cu foam as a plate grid can sustain the structure, and Li-Mg alloy as the active and lithophilic component can guide the uniform Li plating within the composite. Thus, Li-Mg/Cu electrode shows long-term stability in terms of dimensional change and surface morphology. This work provides a facile and practical way to fabricate composite Li electrodes with high dimensional stability for secondary batteries.
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Colloidally grown nanosized semiconductors yield extremely high-quality optoelectronic materials. Many examples have pointed to near perfect photoluminescence quantum yields, allowing for technology-leading materials such as high purity color centers in display technology. Furthermore, because of high chemical yield, and improved understanding of the surfaces, these materials, particularly colloidal quantum dots (QDs) can also be ideal candidates for other optoelectronic applications. Given the urgent necessity toward carbon neutrality, electricity from solar photovoltaics will play a large role in the power generation sector. QDs are developed and shown dramatic improvements over the past 15 years as photoactive materials in photovoltaics with various innovative deposition properties which can lead to exceptionally low-cost and high-performance devices. Once the key issues related to charge transport in optically thick arrays are addressed, QD-based photovoltaic technology can become a better candidate for practical application. In this article, the authors show how the possibilities of different deposition techniques can bring QD-based solar cells to the industrial level and discuss the challenges for perovskite QD solar cells in particular, to achieve large-area fabrication for further advancing technology to solve pivotal energy and environmental issues.
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Lithium-sulfur (Li-S) batteries hold the promise of the next generation energy storage system beyond state-of-the-art lithium-ion batteries. Despite the attractive gravimetric energy density (WG ), the volumetric energy density (WV ) still remains a great challenge for the practical application, based on the primary requirement of Small and Light for Li-S batteries. This review highlights the importance of cathode density, sulfur content, electroactivity in achieving high energy densities. In the first part, key factors are analyzed in a model on negative/positive ratio, cathode design, and electrolyte/sulfur ratio, orientated toward energy densities of 700 Wh L-1 /500 Wh kg-1 . Subsequently, recent progresses on enhancing WV for coin/pouch cells are reviewed primarily on cathode. Especially, the "Three High One Low" (THOL) (high sulfur fraction, high sulfur loading, high density host, and low electrolyte quantity) is proposed as a feasible strategy for achieving high WV , taking high WG into consideration simultaneously. Meanwhile, host materials with desired catalytic activity should be paid more attention for fabricating high performance cathode. In the last part, key engineering technologies on manipulating the cathode porosity/density are discussed, including calendering and dry electrode coating. Finally, a future outlook is provided for enhancing both WV and WG of the Li-S batteries.
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Despite their high theoretical energy density, the application of lithium-sulfur batteries is seriously hindered by the polysulfide shuttle and sluggish kinetics, especially with high sulfur loading and under low electrolyte usage. Herein, to facilitate the conversion of lithium polysulfides, nickel-boron (Ni-B) alloy nanoparticles, dispersed uniformly on carbon nanotube microspheres (CNTMs), are used as sulfur hosts for lithium-sulfur batteries. It is demonstrated that Ni-B alloy nanoparticles can not only anchor polysulfides through Ni-S and B-S interactions but also exhibit high electrocatalytic capability toward the conversion of intermediate polysulfide species. In addition, the intertwined CNT microspheres provide an additional conductive scaffold in response to the fast electrochemical redox. The enhanced redox kinetics is beneficial to improve the specific capacity and cycling stability of the sulfur cathode, based on the fast conversion of lithium polysulfides and effective deposition of the final sulfide products. Conclusively, the S/Ni-B/CNTM composite delivers a high specific capacity (1112.7 mAh gs-1) along with good cycle performance under both high sulfur loading (8.3 mg cm-2) and a lean electrolyte (3 µL mgs-1). Consequently, this study opens up a path to design new sulfur hosts toward lithium-sulfur batteries.
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The high-nickel layered oxides are potential candidate cathode materials of next-generation high energy lithium-ion batteries, in which higher nickel/lower cobalt strategy is effective for increasing specific capacity and reducing cost of cathode. Unfortunately, the fast decay of capacity/potential, and serious thermal concern are critical obstacles for the commercialization of high-nickel oxides due to structural instability. Herein, in order to improve the structure and thermal stability of high-nickel layered oxides, we demonstrate a feasible and simple strategy of the surface gradient doping with yttrium, without forming the hard interface between coating layer and bulk. As expected, after introducing yttrium, the surface gradient doping layer is formed tightly based on the oxidation induced segregation, leading to improved structure and thermal stability. Correspondingly, the good capacity retention and potential stability are obtained for the yttrium-doped sample, together with the superior thermal behavior. The excellent electrochemical performance of the yttrium-doped sample is primarily attributed to the strong yttrium-oxygen bonding and stable oxygen framework on the surface layer. Therefore, the surface manipulating strategy with the surface gradient doping is feasible and effective for improving the structure and thermal stability, as well as the capacity/potential stability during cycling for the high-Ni layered oxides.
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Metallic lithium as an anode is an ultimate ideal for rechargeable lithium batteries with high energy density such as lithium-oxygen batteries and lithium-sulfur batteries. However, the excess reactivity and asymmetrical dissolution-deposition of the metallic lithium anode make it impossible to support a stable long charge-discharge cycling. To protect the metallic lithium anode, apparently it needs to adjust the dissolution and deposition of lithium ions, but more essentially, it should reasonably change the distribution and transport of electrons on the surface and interface of the metallic lithium. In this work, anodic aluminum oxide (AAO) membranes are used to build highly ordered channels on the lithium anode surface in which lithium ions can transfer in the channels and electrons can be transported by the lithiation reaction of alumina with an oxygen vacancy-involved process. As a result, the cyclic reaction actually is partially transferred to the AAO surface, and lithium deposition occurs there as a hemispherical appearance but not as dendrites. Meanwhile, the highly ordered characteristics provide a physical effect to make the deposited lithium hemispheres a uniform distribution on the AAO surface. The AAO-regulated lithium anodes could be widely used to improve the cycling performance for metal lithium batteries.
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Glass-ceramic sulfide solid electrolytes like Li7P3S11 are practicable propellants for safe and high-performance all-solid-state lithium-sulfur batteries (ASSLSBs); however, the stability and conductivity issues remain unsatisfactory. Herein, we propose a congener substitution strategy to optimize Li7P3S11 as Li7P2.9Sb0.1S10.75O0.25 via chemical bond and structure regulation. Specifically, Li7P2.9Sb0.1S10.75O0.25 is obtained by a Sb2O5 dopant to achieve partial Sb/P and O/S substitution. Benefiting from the strengthened oxysulfide structural unit of POS33- and P2OS64- with bridging oxygen atoms and a distorted lattice configuration of the Sb-S tetrahedron, the Li7P2.9Sb0.1S10.75O0.25 electrolyte exhibits prominent chemical stability and high ionic conductivity. Besides the improved air stability, the ionic conductivity of Li7P2.9Sb0.1S10.75O0.25 could reach 1.61 × 10-3 S cm-1 at room temperature with a wide electrochemical window of up to 5 V (vs Li/Li+), as well as good stability against Li and Li-In alloy anodes. Consequently, the ASSLSB with the Li7P2.9Sb0.1S10.75O0.25 electrolyte shows high discharge capacities of 1374.4 mAh g-1 (0.05C, 50th cycle) at room temperature and 1365.4 mAh g-1 (0.1C, 100th cycle) at 60 °C. The battery also presents remarkable rate performance (1158.3 mAh g-1 at 1C) and high Coulombic efficiency (>99.8%). This work provides a feasible technical route for fabricating ASSLSBs.
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The merits of Ni-rich layered oxide cathodes in specific capacity and material cost accelerate their practical applications in electric vehicles and grid energy storage. However, detrimental structural deterioration occurs inevitably during long-term cycling, leading to potential instability and capacity decay of the cathodes. In this work, we investigate the effect of the doped cation radius on the electrochemical performance and structural stability of Ni-rich cathode materials by doping with Mg and Ca ions in LiNi0.8Co0.1Mn0.1O2. The results reveal that an increase in the doping ion radius can enlarge the interlayer spacing but lead to the collapse of the layered structure if the ion radius is too large, which undermines the cycling stability of the cathode material. Compared with the Ca-doped sample and the pristine material, Mg-doped LiNi0.8Co0.1Mn0.1O2 presents improved structural stability and superior thermal stability due to the pillar and glue roles of medium-sized Mg ions in the lithium layer. The results of this study suggest that a suitable ionic radius of the dopant is critical for stabilizing the structure and improving the electrochemical properties of Ni-rich layered oxide cathode materials.
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It is undoubtable that the use of solar energy will continue to increase. Solar cells that convert solar energy directly to electricity are one of the most convenient and important photoelectric conversion devices. Though silicon-based solar cells and thin-film solar cells have been commercialized, developing low-cost and highly efficient solar cells to meet future needs is still a long-term challenge. Some emerging solar-cell types, such as dye-sensitized and perovskite, are approaching acceptable performance levels, but their costs remain too high. To obtain a higher performance-price ratio, it is necessary to find new low-cost counter materials to replace conventional precious metal electrodes (Pt, Au, and Ag) in these emerging solar cells. In recent years, the number of counter-electrode materials available, and their scope for further improvement, has expanded for dye-sensitized and perovskite solar cells. Generally regular patterns in the intrinsic features and structural design of counter materials for emerging solar cells, in particular from an electrochemical perspective and their effects on cost and efficiency, are explored. It is hoped that this recapitulative analysis will help to make clear what has been achieved and what still remains for the development of cost-effective counter-electrode materials in emerging solar cells.
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For high-energy lithium-sulfur batteries, the poor volumetric energy density is a bottleneck as compared with lithium-ion batteries, due to the low density of both the sulfur active material and sulfur host. Herein, in order to enhance the volumetric energy density of sulfur cathode, a universal approach is proposed to fabricate a compact sulfur cathode with dense materials as sulfur host, instead of the old-fashioned lightweight carbon nanomaterials. Based on this strategy, heavy lanthanum strontium manganese oxide (La0.8Sr0.2MnO3), with a high theoretical density of up to 6.5 g cm-3, is introduced as sulfur host. Meanwhile, the La0.8Sr0.2MnO3 host also acts as an efficient electrocatalyst to accelerate the diffusion, adsorption, and redox dynamics of lithium polysulfides in the charge-discharge processes. As a result, such S/La0.8Sr0.2MnO3 cathode presents high gravimetric/volumetric capacity and outstanding cycling stability. Moreover, an ultra-high volumetric energy density of 2727 Wh L-1 -cathode is achieved based on the densification effect with higher density (1.69 g cm-3), which is competitive to the Ni-rich oxide cathode (1800-2160 Wh L-1) of lithium-ion batteries. The current study opens up a path for constructing high volumetric capacity sulfur cathode with heavy and catalytic host toward practical applications of lithium-sulfur batteries.
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Li-rich layered oxide cathode materials are regarded as an attractive candidate of next-generation Li-ion batteries (LIBs) to realize an energy density of >300 Wh kg-1. However, challenges such as capacity fade, cycle life, oxygen release, and structural transformation still restrain its practical application. Micro/nanotechnology is one of the effective strategies to enhance its structural stability and electrochemical performance. An in-depth understanding of the relationship between micro/nanostructures and the electrochemical performance of Li-rich layered oxides is undoubtedly important for developing high-performance cathode materials. Herein, Li1.2Ni0.13Co0.13Mn0.54O2 with different micro/nanostructures including irregular particles, microspheres, microrods, and orthogonal particles are synthesized. Starting from the amount of surface oxygen vacancies in the different structures, the influence of oxygen vacancies on every step during the charge-discharge processes is analyzed by experimental characterizations and theoretical calculations. It is indicated that intrinsic oxygen vacancies can enhance the electrical conductivity and decrease the energy barrier for ion migration, which exerts a significant influence on promoting the kinetics and capacity. Among the different micro/nanostructures, microrods with abundant oxygen vacancies can not only promote lithium ion transport but also stabilize a cathode electrolyte interface (CEI) film by adjusting the distribution of surface elements with lower nickel content. The microrods deliver an initial discharge capacity of up to 306.1 mAh g-1 at 0.1C rate and a superior cycle performance with a capacity retention of 91.0% after 200 cycles at 0.2C rate.
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Effective hosts of sulfur are essential for the application of lithium-sulfur batteries. However, various refined nanomaterials or carbon-based hosts possess low density, high surface area, and large porosity, leading to undesirable reduction on both gravimetric and volumetric energy densities. Herein, spherical metal oxides with high tap density are introduced as carbon-free hosts of sulfur for the first time. The ternary oxides show a superior synergistic effect of adsorption and electrocatalytic conversion of soluble intermediate polysulfides. Besides, oxide microspheres can build stable conductive frameworks and open channels in porous electrodes for fast transport of electrons and active diffusion of electrolyte. Such a synergistic effect and unique structural feature of porous electrodes are favorable for achieving good utilization and stable cycle performance of the sulfur cathode. Typically, the S/LiNi0.8Co0.1Mn0.1O2 composite exhibits good cycle stability with a low capacity decay rate (0.057% per cycle) during 500 cycles at 0.1 C. Importantly, due to the high tap density (1.81 g cm-3), the S/LiNi0.8Co0.1Mn0.1O2 composite delivers a larger volumetric capacity (1601.9 mAh cm-3-composite), almost 2.3 times of S/carbon composite (689.4 mAh cm-3-composite). Therefore, this work provides a feasible strategy to reach long life and high volumetric capacity of cathode based on metal oxides as sulfur hosts.
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Solar cells and rechargeable batteries are two key technologies for energy conversion and storage in modern society. Here, an integrated solar-driven rechargeable lithium-sulfur battery system using a joint carbon electrode in one structure unit is proposed. Specifically, three perovskite solar cells are assembled serially in a single substrate to photocharge a high energy lithium-sulfur (Li-S) battery, accompanied by direct conversion of the solar energy to chemical energy. In the subsequent discharge process, the chemical energy stored in the Li-S battery is further converted to electrical energy. Therefore, the newly designed battery is capable of achieving solar-to-chemical energy conversion under solar-driven conditions, and subsequently delivering electrical energy from the stored chemical energy. With an optimized structure design, a high overall energy conversion efficiency of 5.14% is realized for the integrated battery. Moreover, owing to the self-adjusting photocharge advantage, the battery system can retain high specific capacity up to 762.4 mAh g-1 under a high photocharge rate within 30 min, showing an effective photocharging feature.
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High-Ni layered oxides are potential cathodes for high energy Li-ion batteries due to their large specific capacity advantage. However, the fast capacity fade by undesirable structural degradation in liquid electrolyte during long-term cycling is a stumbling block for the commercial application of high-Ni oxides. In this work, a functional gel polymer electrolyte, grafted with sodium alginate, is introduced to increase the stability of high-Ni oxide cathodes at the levels of both the particle and electrode. An in situ generated ion-conducting layer appears on the interface through the chemical interaction between transition-metal cations of the cathode and the metalophilic reticulum group in sodium alginate. Such a tailoring layer can not only enhance the interfacial compatibility on the cathode/electrolyte interface, reducing the interfacial resistance, but also inhibit the HF corrosion, suppressing the dissolution of transition-metal cations and harmful gradient distribution of components through the oxide cathode at the electrode level. Meanwhile, detrimental microcracks in oxide microspheres and between primary crystallites are impressively inhibited at the particle level. The high-Ni oxide cathode with the metalophilic gel polymer electrolyte shows excellent cycle stability with large initial capacity of 204.9 mA h g-1 at a 1.0 C rate and high discharge capacity retention within 300 cycles at high temperature.