Superior Transport Properties Research Articles

Durable and Versatile Immobilized Carbonic Anhydrase on Textile Structured Packing for CO2 Capture

High-performance carbon dioxide (CO2)-capture technologies with low environmental impact are necessary to combat the current climate change crisis. Durable and versatile “drop-in-ready” textile structured packings with covalently immobilized carbonic anhydrase (CA) were created as efficient, easy to handle catalysts for CO2 absorption in benign solvents. The hydrophilic textile structure itself contributed high surface area and superior liquid transport properties to promote gas-liquid reactions that were further enhanced by the presence of CA, leading to excellent CO2 absorption efficiencies in lab-scale tests. Mechanistic investigations revealed that CO2 capture efficiency depended primarily on immobilized enzymes at or near the surface, whereas polymer entrapped enzymes were more protected from external stressors than those exposed at the surface, providing strategies to optimize performance and durability. Textile packing with covalently attached enzyme aggregates retained 100% of the initial 66.7% CO2 capture efficiency over 71-day longevity testing and retained 85% of the initial capture efficiency after 1-year of ambient dry storage. Subsequent stable performance in a 500 h continuous liquid flow scrubber test emphasized the material robustness. Biocatalytic textile packings performed well with different desirable solvents and across wide CO2 concentration ranges that are critical for CO2 capture from coal and natural gas-fired power plants, from natural gas and biogas for fuel upgrading, and directly from air.

Efficient X-ray CT-based numerical computations of structural and mass transport properties of nickel foam-based GDLs for PEFCs

Nickel foams are excellent candidate materials for gas diffusion layers (GDLs) for polymer electrolyte fuel cells (PEFCs) and this is due to their superior structural and transport properties. A highly computationally-efficient framework has been developed to not only estimate the key structural and mass transport properties but also to examine the multi-dimensional uniformity and/or the isotropy of these properties. Specifically, multiple two-dimensional X-ray CT images and/or numerical models have been used to computationally determine the porosity, the tortuosity, the pore size distribution, the ligament thickness, the specific surface area, the gas permeability and the effective diffusivity of a typical nickel foam sample. The results show that, compared to the conventionally used carbon substrate, the nickel foam sample demonstrate a high degree of uniformity and isotropy and that it has superior structural and mass transport properties, thus underpinning its candidacy as a GDL material for PEFCs. All the computationally-estimated properties, which were found to be consistent with the corresponding literature data, have been presented and thoroughly discussed.

Reactive laser interference patterning on titanium and zinc in high pressure CO2

Direct laser interference patterning (DLIP) is a versatile technique for surface patterning that enables formation of micro-nano sized periodic structures on top of the target material. In this study, DLIP in high pressure, supercritical and liquid CO2 by 4-beam DLIP was used to pattern titanium and zinc targets. Field emission scanning electron microscopy, atomic force microscopy, and X-ray photoelectron spectroscopy was used to characterize the patterned surfaces. Field emission SEM analysis showed presence of ordered uniform donut ring pattern with hollow centers for both titanium and zinc with a period slightly under 3 µm while topographical images from atomic force microscopy revealed donut rings protruding outwards typically around 200 nm from target surface and consisted of a crevice at the center with a depth typically around 300 nm and 250 nm for titanium and zinc target, respectively. Based on X-ray photoelectron spectroscopic analysis, this is the first study to report formation of TiO2, TiC, ZnCO3, and zinc hydroxy carbonate on the pattern by DLIP in supercritical and liquid CO2 for titanium and zinc targets. Pressurized CO2 is demonstrated as a promising environment with mirror-based DLIP system for reactive patterning. Due to the superior transport properties and solvent power of supercritical CO2, the current study opens possibilities for reactive patterning in environments that may not have been previously possible.

Polymer‐Wrapped Perovskite Single Crystal for Surface Passivation and Robust Stability

AbstractMetal halide perovskites (MHPs) emerging as a promising semiconducting material have shown superiority in optoelectronic applications. Currently, polycrystalline perovskite thin films are dominantly employed; while owing to the existence of grain boundary, the polycrystalline films typically have charge transport issues. To overcome these limitations, a perovskite single crystal (SC) is synthesized and applied owing to the more superior bulk charge transport properties compared with its polycrystalline counterpart. Nevertheless, due to the defective nature of the crystal surface, the surfaces of single crystals remain the bottleneck that not only induces stability issues but also causes interfacial charge carrier recombination. In this work, triple cation perovskite single crystals, FA0.8MA0.15Cs0.05PbI3 (denoted as FAMACs) are synthesized, and a facile surface modification strategy is reported for single crystals by polymer monolayer coupling, which shows high effectiveness for improving stability and reducing surface trap state density for single crystals. The polymer‐wrapped single crystals exhibit robust stability and a well‐passivated surface, which shows an order of magnitude lower trap density compared with those of unmodified single crystals and achieves a high responsivity of 5.069 A W−1 when used in photodetector applications.

Vertical gradient freeze growth of detector grade CdZnTeSe single crystals

We report the growth of detector grade Cd0.9Zn0.1Te0.97Se0.03 (CZTS) single crystals, a recently discovered quaternary semiconductor for room temperature radiation detection, by a vertical gradient freeze (VGF) method. VGF is a comparatively low-temperature growth method and avoids relative motion between the heater and the ampoule containing the precursor materials which minimizes any thermal drift or temperature fluctuations. As a result, CZTS single crystals with superior charge transport properties has been obtained. Growth of detector-grade CZTS single crystals using VGF method has not been reported yet. X-ray spectroscopy based elemental analysis showed that the grown crystals demonstrated the desired stoichiometry required for high resolution radiation detection. Planar detectors fabricated by deposition of gold contacts (∼0.07 cm2) demonstrated high bulk resistivity ∼1010 Ω-cm and a very low leakage current density of 2.8 × 10−8 A/cm2 at a bias of 100 V when measured at room temperature. The detectors showed excellent radiation response with 100 % charge collection efficiency when exposed to 5486 keV alpha particles. The electron mobility-lifetime (μτ) product was measured to be 3 × 10−3 cm2/V using a single polarity Hecht analysis which is at par with the recently reported values measured in CZTS grown using conventional Bridgman or travelling heater method. The electron mobility has been calculated to be 964 cm2V−1s−1 using a time-of-flight (TOF) method, a substantial improvement over that obtained from conventionally grown CZTS single crystals.

Avoid Pitfalls in Identifying Perovskite Grain Size.

Perovskite grain size has been used as one of the indicators to evaluate the morphological quality of perovskite films. Large grain size is customarily regarded as an indicator of high photovoltaic performance because it is thought to result in superior charge carrier transport properties due to less carrier scattering by the grain boundaries (GBs). Consequently, the characterization of perovskite grain size has become routine in perovskite solar cell research, and large grain size is in general pursued. However, grain size estimation relying on the prevailing methods, such as scanning electron microscopy (SEM), can be viewed only as "apparent grain size", which is incomplete or possibly wrong for evaluating GB distribution. To avoid the pitfalls and advocate for accurate methodologies in identifying perovskite grain size, this Viewpoint highlights the pitfalls by demonstrating specific examples and then provides an appropriate platform to accurately evaluate perovskite grain information.

Modeling Potential and Species Distribution in a Li||Bi Liquid Metal Battery Using the Finite Volume Method

To match the growing demand for grid scale energy storage in order to balance out renewable energies, the liquid metal battery (LMB) technology is highly promising. Key elements of these batteries are the liquid electrodes, which require LMBs operating at elevated temperatures. Hereby, the electrolyte can be liquid or solid state. Based on density differences, the battery is self-assembling since the components self-segregate when the system is heated. Additionally, many of the possible materials are earth-abundant and not expensive. This results in a very cost effective technology. Moreover, the molten electrodes feature superior kinetics and transport properties as well as high voltage efficiencies at high current densities. Otherwise, the liquidity has the disadvantage that high operating temperatures are necessary. Further, there is a risk of corrosion, self-discharge and short-circuiting. The latter makes the battery not applicable for portable applications [Kim, H. et al. Chem. Rev. 113 (3) (2013)]. Among all LMBs, the Li||Bi cell has been investigated to a large extend and therefore, most material properties are readily available. This is the reason why the present study focuses on this material pairing. A schematic of this cell during discharge is shown in figure 1a. Here, the anode metal Lithium is oxidized and the ion crosses the electrolyte layer. Then it alloys with the molten Bismuth. At charge, this process is reversed. A picture of a real cell can be found in figure 1b. Nevertheless, there are other very promising cell chemistries such as NaZn batteries [Xu, J. et al. J. Power Sources 332 (2016)].For theoretical investigations and numerical simulations, electromagnetic fields, electrochemistry and fluid dynamics need to be considered. Coupling of the corresponding fundamental equations and the different regions in the battery is challenging. Further, there are multiple fluid flow phenomena – like surface instabilities, Tayler instability, electro-vortex flow, thermal convection,solutal convection or Marangoni convection [Kelley, D. H. and Weier, T. Appl. Mech. Rev. 70 (2) (2018)] – that might occur when the battery is operated. To determine the operating voltage of a cell, overpotentials need to be investigated. Generally, there are three types of overpotentials: the ohmic loss, the mass transfer and the charge transfer overpotential. However, the latter can be neglected [Newhouse, J. M. Ph.D. thesis, MIT (2014)]. Determining the ohmic overpotential is quite straightforward using Ohm’s law, while the concentration overpotential requires the calculation of the species distribution in the electrolyte and the positive electrode.The present study will focus on the electrochemical behavior of an all liquid Li||Bi battery and neglects fluid flow. Hereby, the whole cell is modeled using the parent-child-mesh technique from Weber et al. [Weber, N. et al. Computers & Fluids 168 (2018)]. This implies that the species distribution in the electrolyte and the distribution of the dissolved species in the cathode are calculated locally and the potential and current density distribution are calculated globally. The equations to solve are coupled between the used meshes. To account for the potential distribution, it is necessary to consider the electrochemical double layer at the electrode-electrolyte interfaces. Macroscopically, the latter can be described as a potential jump at both interfaces in accordance to the Nernst equation. Weber et al. [Weber, N. et al. Electrochim. Acta 318 (2019)] introduced to model this jump using a source term. In the present study, the approach to use internal jump boundary conditions for modeling the potential jump is proposed. To the best knowledge of the authors, species distributions in the electrolyte have not been investigated previously. When there is no mixing of the electrolyte of LMBs, concentration gradients of each species might be significant [Vallet, C. E. et al. J. Electrochem. Soc. 130 (12) (1983)]. Based on the solution for the species distribution, the potential jump at each interface can be calculated. Further, the charge transfer overpotentials can be obtained.The equations are solved quasi-one-dimensional using the finite volume method and are implemented in the open source library OpenFOAM. To validate this new approach, a comparative study with Comsol is performed. Lastly, an application case is simulated, which confirms that concentration layers in the electrolyte are indeed present. This is, for the case of an Li+ ion in a LiCl-KCl eutectic molten salt, exemplarily shown in figure 1d. Further, as it can be seen in figure 1c, the simulation is able to solve the potential distribution in the cell with respect to the potential jump at the interface.Acknowledgment: This project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No 963599. Figure 1

(Invited) Light Driven H2 Generation in Pt-Tipped CdS Nanorods: Dependence on the Pt Size and CdS Rod Length

Colloidal quantum confined semiconductor-metal nano-heterostructures are a promising class of photocatalysts for solar energy conversion. In these photocatalysts, the semiconductor domain serves as the light absorber and the metal as the catalyst. Such photocatalysts combine the superior light absorption and charge transport properties of the semiconductor with the superior catalytic activity and selectivity of the metal. Furthermore, both domains can be independently tuned to enhance the photocatalytic performance of the heterostructure. Among various semiconductor/metal heterostructures, metal-tipped colloidal semiconductor nanorods (such as CdS-Pt), have attracted extensive interest because they have been reported to have high quantum efficiencies of light driven H2 generation and their morphology can be systematically tuned. The overall light driven H2 generation process involves multiple elementary charge separation and recombination steps in the semiconductor and across the semiconductor/metal interface as well as proton-coupled electron transfer reactions at the catalytic center. The change of the semiconductor or metal domains can often have effects on multiple competing processes involved in the overall reaction. As a result of these complexities, the mechanisms for the morphological dependence of the observed H2 generation efficiencies are not fully understood, hindering the rational design of these photocatalysts. In this talk, we use Pt tipped CdS nanorods (CdS-Pt) as a model system to examine the effect of Pt size and CdS rod length on their light driven H2 generation efficiency. We show that increasing the Pt particle size increases the overall H2 generation quantum efficiency through both increasing the rate of electron transfer from the CdS to Pt and enhancing the efficiency of water/proton reduction; H2 generation efficiency increases at longer CdS rod length by suppression of charge recombination across the Pt/CdS interface. Our work demonstrates that through systematic in situ study of elementary processes involved in the overall H2 generation, it is possible to rationally design and improve semiconductor-metal hybrid photocatalysts.

Anodic WO3 layers sensitized with hematite operating under the visible light spectrum

Tungsten oxide has been considered one of the most promising photoanode materials for photoelectrochemical (PEC) water splitting. WO3 possesses a relatively narrow band gap (2.5–2.8 eV) and superior charge transport properties. In this paper, for the first time, anodic WO3 layers were sensitized with Fe2O3 by electrodeposition and re-annealing method. The influence of FeCl3 concentration in the electrolyte used for the electrodeposition process on the morphology, semiconducting and photoelectrochemical properties was investigated. Since the band gap of hematite is narrower when compared to tungsten oxide, its modification/sensitization with hematite is a promising way to transfer WO3 photoactivity to the visible light region. To sum up, a successfully performed synthesis of Fe2O3-WO3 and Fe2O3–C,N-WO3 heterojunctions resulted in a shift of the material photoresponse towards the visible light region even to the wavelength of 550 nm. The best results were achieved for the Fe2O3–C,N-WO3 sample, that exhibits IPCE values about 1.6 times higher at 450 nm and 12 times higher at 480 nm in comparison to pristine anodic WO3.

Band-like transport in non-fullerene acceptor semiconductor Y6

The recently reported non-fullerene acceptor (NFA) Y6 has been extensively investigated for high-performance organic solar cells. However, its charge transport property and physics have not been fully studied. In this work, we acquired a deeper understanding of the charge transport in Y6 by fabricating and characterizing thin-film transistors (TFTs), and found that the electron mobility of Y6 is over 0.3–0.4 cm2/(V⋅s) in top-gate bottom-contact devices, which is at least one order of magnitude higher than that of another well-known NFA ITIC. More importantly, we observed band-like transport in Y6 spin-coated films through temperature-dependent measurements on TFTs. This is particularly amazing since such transport behavior is rarely seen in polycrystalline organic semiconductor films. Further morphology characterization and discussions indicate that the band-like transport originates from the unique molecule packing motif of Y6 and the special phase of the film. As such, this work not only demonstrates the superior charge transport property of Y6, but also suggests the great potential of developing high-mobility n-type organic semiconductors, on the basis of Y6.Graphical

Fast evaluation technique for the shear viscosity and ionic conductivity of electrolyte solutions

With the growing need to obtain ideal materials for various applications, there is an increasing interest in computational methods to rapidly and accurately search for materials. Molecular dynamics simulation is one of the successful methods used to investigate liquid electrolytes with high transport properties applied in lithium-ion batteries. However, further reduction in computational cost is required to find a novel material with the desired properties from a large number of combinations. In this study, we demonstrate an effective fast evaluation technique for shear viscosity and ionic conductivity by molecular dynamics simulation for an exhaustive search of electrolyte materials with high transport properties. The proposed model was combined with a short-time correlation function of the stress tensor and empirical relationships to address the issues of inefficient and uncertain evaluation by conventional molecular dynamics methods. Because we focus on liquid electrolytes consisting of organic solvents and lithium salts, our model requires dissociation ratio and effective diffusion size of lithium salts. Our method is applied to search for the compositional combinations of electrolytes with superior transport properties even at low temperatures. These results correlate well with experimental results.

Fast Exciton Diffusion in Monolayer PtSe2

AbstractRecently, 2D noble metal dichalcogenides have drawn considerable attention due to their thickness‐tunable electronic and optical properties. However, the dynamical properties of photocarriers in these materials are less studied. Here, photocarrier dynamics in monolayer and bilayer PtSe samples prepared by chemical vapor deposition are studied by transient absorption microscopy. Spatially and temporally resolved differential reflectance measurements yield room‐temperature exciton lifetimes of 25 and 50 ps for monolayer and bilayer samples, respectively. The exciton diffusion coefficient in monolayer PtSe is found to be as large as 48 cm s. This value is higher than exciton diffusion coefficients of most known monolayer semiconductors. The deduced exciton mobility is close to the theoretical limit of charge carrier mobility of monolayer PtSe. The superior exciton transport property is unique to monolayers, as the exciton diffusion coefficient drops to 6.7 cm s in bilayers PtSe. The novel exciton transport properties, along with its high air stability, make monolayer PtSe an attractive material for ultrathin excitonic devices. These results provide insights on the exciton dynamic properties of 2D PtSe and help develop fundamental understanding on the performance of various optoelectronic devices based on 2D PtSe.

Promoted charge separation and specific surface area via interlacing of N-doped titanium dioxide nanotubes on carbon nitride nanosheets for photocatalytic degradation of Rhodamine B

Abstract Titanium dioxide (TiO2) has been regarded as a promising catalyst owing to its superior charge transport properties in photocatalytic degradation of organic pollutants and photocatalytic hydrogen generation. However, a major bottleneck toward the utilization of TiO2 photocatalysts is inefficient exploitation of visible light and low adsorption behavior. To address this issue, we fabricated a hybrid nanocomposite composed of one-dimensional N-doped TiO2 nanotubes (N-TNTs) and two-dimensional graphitic carbon nitride nanosheets (g-CNNs) to improve photocatalytic behavior. Furthermore, photogenerated electron–hole pairs in the hybrid N-TNT/g-CNN composites were efficiently separated by introducing g-CNNs. In addition, the improved specific surface area provided many active sites, resulting in higher photocatalytic reactions in kinetics. Based on these features, the Rhodamine B photocatalytic degradation efficiency was the highest, ∼85%, under solar-light irradiation in the N-TNT/g-CNN composites (7 wt% of the g-CNN content), which is two times higher than that of the N-TNT. Moreover, excellent durability and stability were observed after four cycles, which can be attributed to the extended optical absorption range and enhanced separation of the photogenerated electron–hole pairs.

Enhancing the Intermolecular Interactions of Ladder-Type Heteroheptacene-Based Nonfullerene Acceptors for Efficient Polymer Solar Cells by Incorporating Asymmetric Side Chains

Enhancing the Intermolecular Interactions of Ladder-Type Heteroheptacene-Based Nonfullerene Acceptors for Efficient Polymer Solar Cells by Incorporating Asymmetric Side Chains

Back Cover: Defect‐Free Alternating Conjugated Polymers Enabled by Room‐ Temperature Stille Polymerization (Angew. Chem. Int. Ed. 16/2022)

Defect-free alternating conjugated polymers were produced by exploring palladium-catalyzed Stille polymerization at room temperature. The selected copolymers demonstrated no homocoupling defects and superior charge transport properties, thus paving the road for the development of plastic electronics. Details of this study are reported by Qinqin Shi, Hui Huang, and co-workers in their Research Article (e202115969).

Effect of fluorine atoms on the dielectric constants, optoelectronic properties and charge carrier kinetic characteristics of indacenodithieno[3,2-b]thiophene based non-fullerene acceptors for efficient organic solar cells

In this work, the optical and electrochemical properties, charge mobility, the dielectric constants, photovoltaic performance of three non-fullerene acceptors (NFAs) named ITOR-IC, ITOR4F-IC, and ITOR-IC4F, in which 4-octyloxy-phenyl and 3-fluoro-4-octyloxy-phenyl side-chains were connected on the indacenodithieno[3,2-b]thiophene (IT) core and ended with 2-(3-oxo-indane-1-ylidene)-malononitrile or 2–3-(oxo-5,6-difluoro-indane-1-ylidene)-malononitrile end groups, were systematically investigated. It has been found that ITOR-IC4F which ended up with 2–3-(oxo-5,6-difluoro-indane-1-ylidene)-malononitrile groups, exhibited the narrowest bandgap and the highest dielectric constant of 5.10 as compared with that of ITOR-IC (4.03 at 1 kHz) and ITOR4F-IC (4.46 at 1 kHz). Moreover, the PM6:ITOR-IC4F based polymer solar cells (PSCs) presented the highest exciton dissociation probability, superior charge transport and extraction properties, combined with the longest carrier lifetime and the lowest recombination rate coefficient, eventually achieved the highest PCE of 11.1%. The results indicate that the introduction of fluorine atoms into end groups rather than side-chains of the NFAs is more conducive to increasing the dielectric constant of the IT-based NFA, more importantly, improving the photoresponse and the morphology of the active layer, thus devoting to the improvement of the light harvesting, exciton dissociation, as well as the carrier lifetime in the active layer. This work brings forward a new aspect to understand the influence of fluorine atoms substituent position on the properties of the NFAs for the further designation and optimization of new NFAs for efficient PSCs.

Electric Transport Properties of NaAlB14 with Covalent Frameworks.

A synthetic protocol was developed for obtaining a single phase of polycrystalline NaAlB14 with strongly connected intergrain boundaries. NaAlB14 has a unique crystal structure with a tunnel-like covalent framework of B that traps monovalent Na and trivalent Al ions. Owing to the atmospheric instability and volatility of Na, the synthesis of polycrystalline NaAlB14 and its physical properties have not been reported yet. This study employed a two-step process to achieve single-phase polycrystalline NaAlB14. As a first step, a mixture of Al and B with excess Al was sintered in the Na vapor atmosphere followed by HCl treatment to remove excess Al as a second step. For obtaining bulk samples with strong grain connection, vacuum or high-pressure (HP) annealing was employed. HP annealing promoted bandgap shrinkage due to the crystal strain and defect levels and suppressed intergranular resistance. As a result, the HP-annealed sample achieved superior transport properties (0.1 kΩ cm at 300 K) to the vacuum-annealed sample (260 kΩ cm). Furthermore, from the viewpoint of its crystal structure and DFT calculations, the most probable site for the defect was suggested to be the Na site.

Small Size, Big Impact: Recent Progress in Bottom-Up Synthesized Nanographenes for Optoelectronic and Energy Applications.

Bottom‐up synthesized graphene nanostructures, including 0D graphene quantum dots and 1D graphene nanoribbons, have recently emerged as promising candidates for efficient, green optoelectronic, and energy storage applications. The versatility in their molecular structures offers a large and novel library of nanographenes with excellent and adjustable optical, electronic, and catalytic properties. In this minireview, recent progress on the fundamental understanding of the properties of different graphene nanostructures, and their state‐of‐the‐art applications in optoelectronics and energy storage are summarized. The properties of pristine nanographenes, including high emissivity and intriguing blinking effect in graphene quantum dots, superior charge transport properties in graphene nanoribbons, and edge‐specific electrochemistry in various graphene nanostructures, are highlighted. Furthermore, it is shown that emerging nanographene‐2D material‐based van der Waals heterostructures provide an exciting opportunity for efficient green optoelectronics with tunable characteristics. Finally, challenges and opportunities of the field are highlighted by offering guidelines for future combined efforts in the synthesis, assembly, spectroscopic, and electrical studies as well as (nano)fabrication to boost the progress toward advanced device applications.

High directional water transport graphene oxide biphilic stack

ABSTRACT It is a widely held view that the hydrophilicity of graphene oxide (GO) enhances the water transport properties. In this study, it is shown that a combination of graphene and GO can yield superior transport properties including high mass flow rate and directionality. First, different membrane characteristics such as the smallest pore diameter for water molecules sieving and mass flow rate are evaluated. Furthermore, a combination of graphene and GO, a biphilic stack of hydrophobic and hydrophilic layers, is used to evaluate the mass flow rates and results are compared with that of normal GO laminates. This structure acts as a water diode i.e. conducts water molecules in the desired direction and increases the mass flow rate several times. The effects of interatomic potential, oxidation level and charge, and the spacing between layers on mass flow rate and directionality are examined. It is found that an optimized structure conducts water in the desired direction and increases mass flow rate up to 10 times for small interlayer distance of 7 Å compared with normal GO laminates. The given structures can be used in a wide range of filtration applications, where selective water sieving with a high mass flow rate is desired.

Super-structured defects modulation for synergistically optimizing thermoelectric property in SnTe-based materials

Among the intriguing p-type thermoelectric IV-VI compounds, SnTe is an important alternative to both PbTe and GeTe for free of toxicity of Pb and scarcity of Ge. However, pristine SnTe has poor thermoelectric performance because of its intrinsic high hole concentration, big energy difference between L and Σ bands and high lattice thermal conductivity. In this work, In and Cd co-doping SnTe material, which combines the effect of resonant level and band convergence together, was obtained by self-propagating high-temperature synthesis (SHS) and plasma activated sintering (PAS). The generated Te vacancies are regularly arranged to form super-structured defects in the subsequent constrained hot compressing process, which include regular array of atomic defects and nanoscale precipitates. As a result, the hole concentration of the compressed SnTe-based material is reduced due to the donor doping effect of Te vacancies, and the hole mobility is remarkably improved to 372.94 cm2V−1s−1 and 66.19 cm2V−1s−1 at room temperature for the SnTe and In0.01Cd0.02Sn0.97Te material with compressibility of 35%, respectively. These atomic and nanoscale super-structured defects not only ensure superior electrical transport properties, but also bring much stronger scattering effect on phonons, thus leading to extremely low lattice thermal conductivity of 1.2 Wm−1K−1 at 888 K for the 35% compressed In0.01Cd0.02Sn0.97Te material. With synergistically optimized carrier and phonon transport behavior through resonant level engineering, band convergence engineering and super-structured defects engineering, a peak ZT value of 0.8 is achieved in In0.01Cd0.02Sn0.97Te material with compressibility of 35%. This work provides an effective strategy to realize the decoupling of electron and phonon scattering through Te vacancy-based super-structured defects modulation, and makes up an important part of multiscale microstructure tailoring for thermoelectric materials.