Carbon-Based Nanocages: A New Platform for Advanced Energy Storage and Conversion

Energy storage and conversion play a crucial role in modern energy systems, and the exploration of advanced electrode materials is vital but challenging. Carbon-based nanocages consisting of sp² carbon shells feature a hollow interior cavity with sub-nanometer microchannels across the shells, high specific surface area with a defective outer surface, and tunable electronic structure, much different from the intensively studied nanocarbons such as carbon nanotubes and graphene. These structural and morphological characteristics make carbon-based nanocages a new platform for advanced energy storage and conversion. Up-to-date synthetic strategies of carbon-based nanocages, the utilization of their unique porous structure and morphology for the construction of composites with foreign active species, and their significant applications to the advanced energy storage and conversion are reviewed. Structure–performance correlations are discussed in depth to highlight the contribution of carbon-based nanocages. The research challenges and trends are also envisaged for deepening and extending the study and application of this multifunctional material.     

Multifunctional Energy Storage and Conversion Devices

Multifunctional energy storage and conversion devices that incorporate novel features and functions in intelligent and interactive modes, represent a radical advance in consumer products, such as wearable electronics, healthcare devices, artificial intelligence, electric vehicles, smart household, and space satellites, etc. Here, smart energy devices are defined to be energy devices that are responsive to changes in configurational integrity, voltage, mechanical deformation, light, and temperature, called self‐healability, electrochromism, shape memory, photodetection, and thermal responsivity. Advisable materials, device designs, and performances are crucial for the development of energy electronics endowed with these smart functions. Integrating these smart functions in energy storage and conversion devices gives rise to great challenges from the viewpoint of both understanding the fundamental mechanisms and practical implementation. Current state‐of‐art examples of these smart multifunctional energy devices, pertinent to materials, fabrication strategies, and performances, are highlighted. In addition, current challenges and potential solutions from materials synthesis to device performances are discussed. Finally, some important directions in this fast developing field are considered to further expand their application.     

Review on Recent Progress of All‐Inorganic Metal Halide Perovskites and Solar Cells

All‐inorganic perovskites are considered to be one of the most appealing research hotspots in the field of perovskite photovoltaics in the past 3 years due to their superior thermal stability compared to their organic–inorganic hybrid counterparts. The power‐conversion efficiency has reached 17.06% and the number of important publications is ever increasing. Here, the progress of inorganic perovskites is systematically highlighted, covering materials design, preparation of high‐quality perovskite films, and avoidance of phase instabilities. Inorganic perovskites, nanocrystals, quantum dots, and lead‐free compounds are discussed and the corresponding device performances are reviewed, which have been realized on both rigid and flexible substrates. Methods for stabilization of the cubic phase of low‐bandgap inorganic perovskites are emphasized, which is a prerequisite for highly efficient and stable solar cells. In addition, energy loss mechanisms both in the bulk of the perovskite and at the interfaces of perovskite and charge selective layers are unraveled. Reported approaches to reduce these charge‐carrier recombination losses are summarized and complemented by methods proposed from our side. Finally, the potential of inorganic perovskites as stable absorbers is assessed, which opens up new perspectives toward the commercialization of inorganic perovskite solar cells.     

2D Black Phosphorus for Energy Storage and Thermoelectric Applications

Recent progress in the currently available methods of producing black phosphorus bulk and phosphorene are presented. The effective passivation approaches toward improving the air stability of phosphorene are also discussed. Furthermore, the research efforts on the phosphorene and phosphorene‐based materials for potential applications in lithium ion batteries, sodium ion batteries, and thermoelectric devices are summarized and highlighted. Finally, the outlook including challenges and opportunities in these research fields are discussed.     

Lead‐Free Organic–Inorganic Hybrid Perovskites for Photovoltaic Applications: Recent Advances and Perspectives

Organic–inorganic hybrid halide perovskites (e.g., MAPbI₃) have recently emerged as novel active materials for photovoltaic applications with power conversion efficiency over 22%. Conventional perovskite solar cells (PSCs); however, suffer the issue that lead is toxic to the environment and organisms for a long time and is hard to excrete from the body. Therefore, it is imperative to find environmentally‐friendly metal ions to replace lead for the further development of PSCs. Previous work has demonstrated that Sn, Ge, Cu, Bi, and Sb ions could be used as alternative ions in perovskite configurations to form a new environmentally‐friendly lead‐free perovskite structure. Here, we review recent progress on lead‐free PSCs in terms of the theoretical insight and experimental explorations of the crystal structure of lead‐free perovskite, thin film deposition, and device performance. We also discuss the importance of obtaining further understanding of the fundamental properties of lead‐free hybrid perovskites, especially those related to photophysics.     

Gel Electrocatalysts: An Emerging Material Platform for Electrochemical Energy Conversion

Seeking sustainable and cost-effective energy sources is one of the significant challenges for the sustainable development of modern society. To date, considerable expectations have been held for technologies, such as fuel cells and electrolyzers, where the performance strongly depends on electrochemical conversion processes that can generate and store chemical energy through the breaking or formation of chemical bonds. However, those advanced technologies are severely limited by the efficiency, selectivity, and durability of electrocatalysis. Thanks to their hierarchically porous architecture, compositional and structural tunability, and ease of functionalization, the family of gel materials opens exciting opportunities for advanced energy technologies. Unique advances in gel materials based on controllable compositions and functions enable gel electrocatalysts to potentially break the limitations of current materials, enhancing the device performance of electrochemical energy. Here, recent developments and challenges for nanostructured gel-based materials for electrocatalysis applications are summarized. Future possibilities and challenges for gel electrocatalysts in terms of synthesis and applications are also discussed.     

Complex Hydrides for Energy Storage,Conversion, and Utilization

Functional materials are the key enabling factor in the development of clean energy technologies. Materials of particular interest, which are reviewed herein, are a class of hydrogenous compound having the general formula of M(XH_n)_m, where M is usually a metal cation and X can be Al, B, C, N, O, transition metal (TM), or a mixture of them, which sets up an iono‐covalent or covalent bonding with H. M(XH_n)_m is generally termed as a complex hydride by the hydrogen storage community. The rich chemistry between H and B/C/N/O/Al/TM allows complex hydrides of diverse composition and electronic configuration, and thus tunable physical and chemical properties, for applications in hydrogen storage, thermal energy storage, ion conduction in electrochemical devices, and catalysis in fuel processing. The recent progress is reviewed here and strategic approaches for the design and optimization of complex hydrides for the abovementioned applications are highlighted.     

Superior Energy Storage Capability and Stability in Lead-Free Relaxors for Dielectric Capacitors Utilizing Nanoscale Polarization Heterogeneous Regions

The development of high-performance lead-free dielectric ceramic capacitors is essential in the field of advanced electronics and electrical power systems. A huge challenge, however, is how to simultaneously realize large recoverable energy density (W_rec), ultrahigh efficiency (η), and satisfactory temperature stability to effectuate next-generation high/pulsed power capacitors applications. Here, a strategy of utilizing nanoscale polarization heterogeneous regions is demonstrated for high-performance dielectric capacitors, showing comprehensive properties of large W_rec (≈6.39 J cm⁻³) and ultrahigh η (≈94.4%) at 700 kV cm⁻¹ accompanied by excellent thermal endurance (20–160 °C), frequency stability (5–200 Hz), cycling reliability (1–105 cycles) at 500 kV cm⁻¹, and superior charging-discharging performance (discharge rate t_0.9 ≈ 28.4 ns, power density PD ≈161.3 MW cm⁻³). The observations reveal that constructing the polarization heterogeneous regions in a linear dielectric to form novel relaxor ferroelectrics produces favorable microstructural characters, including extremely small polar nanoregions with high dynamics and multiphase coexistence and stable local structure symmetry, which enables large breakdown strength and ultralow polarization switching hysteresis, hence synergistically contributing to high-efficient capacitive energy storage. This study thus opens up a novel strategy to design lead-free dielectrics with comprehensive high-efficient energy storage performance for advanced pulsed power capacitors applications.     

Polymer‐Passivated Inorganic Cesium Lead Mixed‐Halide Perovskites for Stable and Efficient Solar Cells with High Open‐Circuit Voltage over 1.3 V

Cesium‐based trihalide perovskites have been demonstrated as promising light absorbers for photovoltaic applications due to their superb composition stability. However, the large energy losses (E_loss) observed in inorganic perovskite solar cells has become a major hindrance impairing the ultimate efficiency. Here, an effective and reproducible method of modifying the interface between a CsPbI₂Br absorber and polythiophene hole‐acceptor to minimize the E_loss is reported. It is demonstrated that polythiophene, deposited on the top of CsPbI₂Br, can significantly reduce electron‐hole recombination within the perovskite, which is due to the electronic passivation of surface defect states. In addition, the interfacial properties are improved by a simple annealing process, leading to significantly reduced energy disorder in polythiophene and enhanced hole‐injection into the hole‐acceptor. Consequently, one of the highest power conversion efficiency (PCE) of 12.02% from a reverse scan in inorganic mixed‐halide perovskite solar cells is obtained. Modifying the perovskite films with annealing polythiophene enables an open‐circuit voltage (V_OC) of up to 1.32 V and E_loss of down to 0.5 eV, which both are the optimal values reported among cesium‐lead mixed‐halide perovskite solar cells to date. This method provides a new route to further improve the efficiency of perovskite solar cells by minimizing the E_loss.     

2D Superlattices for Efficient Energy Storage and Conversion

2D genuine unilamellar nanosheets, that are, the elementary building blocks of their layered parent crystals, have gained increasing attention, owing to their unique physical and chemical properties, and 2D features. In parallel with the great efforts to isolate these atomic-thin crystals, a unique strategy to integrate them into 2D vertically stacked heterostuctures has enabled many functional applications. In particular, such 2D heterostructures have recently exhibited numerous exciting electrochemical performances for energy storage and conversion, especially the molecular-scale heteroassembled superlattices using diverse 2D unilamellar nanosheets as building blocks. Herein, the research progress in scalable synthesis of 2D superlattices with an emphasis on a facile solution-phase flocculation method is summarized. A particular focus is brought to the advantages of these 2D superlattices in applications of supercapacitors, rechargeable batteries, and water-splitting catalysis. The challenges and perspectives on this promising field are also outlined.     

Nonsiliceous Mesoporous Materials: Design and Applications in Energy Conversion and Storage

In this work, the progress in the design of nonsiliceous mesoporous materials (nonSiMPMs) over the last five years from the perspectives of the chemical composition, morphology, loading, and surface modification is summarized. Carbon, metal, and metal oxide are in focus, which are the most promising compositions. Then, representative applications of nonSiMPMs are demonstrated in energy conversion and storage, including recent technical advances in dye‐sensitized solar cells, perovskite solar cells, photocatalysts, electrocatalysts, fuel cells, storage batteries, supercapacitors, and hydrogen storage systems. Finally, the requirements and challenges of the design and application of nonSiMPMs are outlined.     

Metallic MoS2 for High Performance Energy Storage and Energy Conversion

Metallic phase 2D molybdenum disulfide (MoS₂) is an emerging class of materials with remarkably higher electrical conductivity and catalytic activities. The goal of this study is to review the atomic structures and electrochemistry of metallic MoS₂, which is essential for a wide range of existing and new enabling technologies. The scope of this paper ranges from the atomic structure, band structure, electrical and optical properties to fabrication methods, and major emerging applications in electrochemical energy storage and energy conversion. This paper also thoroughly covers the atomic structure–properties–application relationships of metallic MoS₂. Understanding the fundamental properties of these structures is crucial for designing and manufacturing products for emerging applications. Today, a more holistic understanding of the interplay between the structure, chemistry, and performance of metallic MoS₂ is advancing actual applications of this material. This new level of understanding also enables a myriad of new and exciting applications, which motivated this review. There are excellent reviews already on the traditional semiconducting MoS₂, and this review, for the first time, focuses on the uniqueness of conducting metallic MoS₂ for energy applications and offers brand new materials for clean energy application.     

Porous Graphene Materials for Advanced Electrochemical Energy Storage and Conversion Devices

Combining the advantages from both porous materials and graphene, porous graphene materials have attracted vast interests due to their large surface areas, unique porous structures, diversified compositions and excellent electronic conductivity. These unordinary features enable porous graphene materials to serve as key components in high‐performance electrochemical energy storage and conversion devices such as lithium ion batteries, supercapacitors, and fuel cells. This progress report summarizes the typical fabrication methods for porous graphene materials with micro‐, meso‐, and macro‐porous structures. The structure–property relationships of these materials and their application in advanced electrochemical devices are also discussed.     

Rational Design of Carbon‐Rich Materials for Energy Storage and Conversion

Carbon‐rich materials have drawn tremendous attention toward a wide spectrum of energy applications due to their superior electronic mobility, good mechanical strength, ultrahigh surface area, and more importantly, abundant diversity in structure and components. Herein, rationally designed and bottom‐up constructed carbon‐rich materials for energy storage and conversion are discussed. The fundamental design principles are itemized for the targeted preparation of carbon‐rich materials and the latest remarkable advances are summarized in terms of emerging dimensions including sp² carbon fragment manipulation, pore structure modulation, topological defect engineering, heteroatom incorporation, and edge chemical regulation. In this respect, the corresponding structure–property relationships of the resultant carbon‐rich materials are comprehensively discussed. Finally, critical perspectives on future challenges of carbon‐rich materials are presented. The progress highlighted here will provide meaningful guidance on the precise design and targeted synthesis of carbon‐rich materials, which are of critical importance for the achievement of performance characteristics highly desirable for urgent energy deployment.     

A Bistable Triboelectric Nanogenerator for Low-Grade Thermal Energy Harvesting and Solar Thermal Energy Conversion

Converting ubiquitous ambient low-grade thermal energy into electricity is of great significance for tackling the fossil energy shortage and environmental crisis but poses a considerable challenge. Here, a novel thermal-driven triboelectric nanogenerator (TD-TENG) is developed, which utilizes a bimetallic beam with a bi-stable dynamic feature to induce continuous mechanical oscillations, and the mechanical motion is then converted into electric power using a contact-separation TENG. The thermal process inside the device is systematically investigated and effective thermal management is conducted accordingly. After optimization, the TD-TENG can produce a power density of 323.9 mW m⁻² at 59.5 °C, obtaining the highest record of TENG-based thermal energy harvesters. Besides, the first prototype of TENG-based solar thermal harvester is successfully demonstrated, with a power density of 364.4 mW m⁻². Moreover, the TD-TENG can harvest and dissipate the heat at the same time, exhibiting great potential in over-heated electronics protection as well as architectural energy conservation. Most importantly, the operation temperature range of the TD-TENG is tunable by adjusting the bimetal parameters, allowing the device a wide and flexible working thermal gradient. These unique properties validate the TD-TENG is a simple, feasible, cost-effective, and high-efficient low-grade thermal energy harvester.