The long-standing popularity of thermoelectric materials has contributed to the creation of various thermoelectric devices and stimulated the development of strategies to improve their thermoelectric performance. In this review, we aim to comprehensively summarize the state-of-the-art strategies for the realization of high-performance thermoelectric materials and devices by establishing the links between synthesis, structural characteristics, properties, underlying chemistry and physics, including structural design (point defects, dislocations, interfaces, inclusions, and pores), multidimensional design (quantum dots/wires, nanoparticles, nanowires, nano- or microbelts, few-layered nanosheets, nano- or microplates, thin films, single crystals, and polycrystalline bulks), and advanced device design (thermoelectric modules, miniature generators and coolers, and flexible thermoelectric generators). The outline of each strategy starts with a concise presentation of their fundamentals and carefully selected examples. In the end, we point out the controversies, challenges, and outlooks toward the future development of thermoelectric materials and devices. Overall, this review will serve to help materials scientists, chemists, and physicists, particularly students and young researchers, in selecting suitable strategies for the improvement of thermoelectrics and potentially other relevant energy conversion technologies.

Advanced Thermoelectric Design: From Materials and Structures to Devices

Research interest in the development of real-time monitoring of personal health indicators using wearable electrocardiographic systems has intensified in recent years. New advanced thermoelectrics are potentially a key enabling technology that can be used to transform human body heat into power for use in wearable electrographic monitoring devices. This work provides a systematic review of the potential application of thermoelectric generators for use as power sources in wearable electrocardiographic monitoring systems. New strategies on miniaturized rigid thermoelectric modules combined with batteries or supercapacitors can provide adequate power supply for wearable electrocardiographic systems. Flexible thermoelectric generators can also support wearable electrocardiographic systems directly when a heat sink is incorporated into the design in order to enlarge and stabilize the temperature gradient. Recent advances in enhancing the performance of novel fiber/fabric based flexible thermoelectrics has opened up an exciting direction for the development of wearable electrocardiographic systems.

Thermoelectric Generators: Alternative Power Supply for Wearable Electrocardiographic Systems.

As an emission-free energy conversion technology, thermoelectric technology has been considered an essential component in solving the global energy crisis. Carbon allotrope hybrids, with relatively low cost, high performance and engineerable mechanical strength and flexibility, are attracting increasing research interest. The key challenge of developing carbon allotrope hybrid thermoelectric applications lies in material performance enhancement, which is further restricted by enhancing the electrical performance, refraining the lattice thermal conductivity and engineering the mechanical properties. Compositing carbon allotropes to enhance electrical transport properties should be mainly attributed to the material orientation effect which increases the carrier mobility or to the energy filtering effect which increases the Seebeck coefficient. The reduced lattice thermal conductivity due to the formation of carbon allotrope hybrid is derived from various additional phonon scattering features. Furthermore, carbon allotrope-compositing is also effective in enhancing the mechanical properties of thermoelectric materials, which can potentially further widen the variety of applications of these materials. A key opportunity in better utilizing the flexibility of carbon materials is deploying them as stents. Carbon allotrope hybrids can provide a pathway such that rigid thermoelectric materials can be designed into flexible thermoelectric materials. Finally, we point out future research directions for carbon-hybrid thermoelectric materials.

Carbon allotrope hybrids advance thermoelectric development and applications

The pillars of Green Chemistry necessitate the development of new chemical methodologies and processes that can benefit chemical synthesis in terms of energy efficiency, conservation of resources, product selectivity, operational simplicity and, crucially, health, safety, and environmental impact. Implementation of green principles whenever possible can spur the growth of benign scientific technologies by considering environmental, economical, and societal sustainability in parallel. These principles seem especially important in the context of the manufacture of materials for sustainable energy and environmental applications. In this review, the production of energy conversion materials is taken as an exemplar, by examining the recent growth in the energy‐efficient synthesis of thermoelectric nanomaterials for use in devices for thermal energy harvesting. Specifically, “soft chemistry” techniques such as solution‐based, solvothermal, microwave‐assisted, and mechanochemical (ball‐milling) methods as viable and sustainable alternatives to processes performed at high temperature and/or pressure are focused. How some of these new approaches are also considered to thermoelectric materials fabrication can influence the properties and performance of the nanomaterials so‐produced and the prospects of developing such techniques further.

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Energy‐Saving Pathways for Thermoelectric Nanomaterial Synthesis: Hydrothermal/Solvothermal, Microwave‐Assisted, Solution‐Based, and Powder Processing

Thermoelectrics can directly harvest electricity from waste heat through the Seebeck effect, therefore it has been regarded as an eco-friendly and sustainable solution to alleviate the pressure from fossil fuel consumption and environmental pollution. Rational structural manipulation is critical to improving the thermoelectric performance of materials, and a timely review is required to summarize the recent progress on the novel structural design for thermoelectrics. In this review, taking SnSe as a typical example and combined with other thermoelectric materials, we summarize recent advances in the rational structural manipulation for thermoelectric materials, including point defects, dislocations, boundaries, nanoinclusions, and nanopores. The inherent links between syntheses, characterizations, and thermoelectric properties by tailoring the structures are established. In addition, we discuss the development of nanoscale thermoelectric materials and their potential for applying to flexible thermoelectric devices. This review can guide the design of high-performance thermoelectric materials.

Rational Structure Design and Manipulation Advance SnSe Thermoelectrics

General surfactant-free synthesis of binary silver chalcogenides with tuneable thermoelectric properties

Realizing enhanced thermoelectric properties in Cu2S-alloyed SnSe based composites produced via solution synthesis and sintering

SnTe is proposed to be one intriguing low-toxicity alternative to PbTe. Herein, we report the diminished lattice thermal conductivity (κL) and enhanced zT of SnTe by way of vacancy engineering. (Sn...

Achieving Enhanced Thermoelectric Performance in (SnTe)1-x(Sb2Te3)x and (SnTe)1-y(Sb2Se3)y Synthesized via Solvothermal Reaction and Sintering

Cu2S, consisting of Earth-abundant and eco-friendly elements, is a promising candidate for thermoelectric energy conversion. The stoichiometric Cu2S has intrinsically low thermal conductivity together with meagre electrical conductivity. Herein, in order to improve the electrical properties, we develop a facile solvothermal method for synthesizing a series of Cu2-xS with tunable phase compositions. With reduction in the CuCl/Na2S molar ratio in the solution precursors from 2:1 to 1.75:1, the solvothermal products transform from single-phase Cu2S into Cu2S-Cu1.96S composites, which are preserved in the hot-pressed pellets. The decreased CuCl/Na2S molar ratio results in increased room-temperature Hall carrier concentration, leading to enhanced electrical conductivity. Specifically, the pellet corresponding to the 1.75:1 CuCl/Na2S precursor ratio obtains a power factor of 8.04 μW cm-1 K-2 at 815 K, which is ∼735% of the value obtained by stoichiometric Cu2S. Along with the moderate thermal conductivity, this sample achieves an enhanced zT value of 0.87 at 815 K, representing a ∼250% increase when compared to stoichiometric Cu2S. This study demonstrates an effective strategy in enhancing the thermoelectric performance of solution-synthesized Cu2S-based materials by phase tuning.

Phase Tuning for Enhancing the Thermoelectric Performance of Solution-Synthesized Cu2-xS.

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Papers

General surfactant-free synthesis of binary silver chalcogenides with tuneable thermoelectric properties

Realizing enhanced thermoelectric properties in Cu2S-alloyed SnSe based composites produced via solution synthesis and sintering

Achieving Enhanced Thermoelectric Performance in (SnTe)1-x(Sb2Te3)x and (SnTe)1-y(Sb2Se3)y Synthesized via Solvothermal Reaction and Sintering

Phase Tuning for Enhancing the Thermoelectric Performance of Solution-Synthesized Cu2-xS.