Sb Atoms Research Articles

Highly Reversible Sodium Metal Batteries Enabled by Extraordinary Alloying Reaction of Single‐Atom Antimony

AbstractThe unique coordination configuration of single‐atom materials (SAMs) allows precise reaction control at atomic‐level and a potential of unusual electrochemical reaction. Nevertheless, it is a big challenge to prepare main group element with high loading content. Here, multifield‐regulated synthesis (MRS) technology is utilized to rapidly produce single‐atom antimony (Sb) metal with a high loading of 15 wt.%. Ab initio molecular dynamics simulations reveal the significantly enhanced reaction kinetics of Sb and nitrogen‐doped graphene by multi‐physics field coupling. Compared with common metallic Sb nanoparticles, atomically dispersed Sb displays remarkably improved electrochemical reaction kinetics and stable structure due to the negligible variation of stresses and volume expansion during the pseudocapacitive alloying‐dealloying process. Such extraordinary alloying reaction in well‐dispersed Sb atoms enabling homogeneous ion flow can serve as active nucleation sites for regulating even Na metal nucleation and growth. As a result, copper foil coated with only ≈3 µm thickness of such material exhibits a high Coulombic efficiency of up to 99.99%, an ultra‐low overpotential of 3 mV, and a long lifetime exceeding 2500 h in symmetrical cells. Furthermore, an anode‐free MRS‐SbSA||Na3V2(PO4)3 battery is constructed, which demonstrates exceptionally high energy density (≈362 Wh Kg−1), outstanding rate capability and good cycling stability.

Novel B6P6X (X=As, Sb) monolayers for antiferromagnetic spintronics and hydrogen storage

Embedding foreign atoms into porous two-dimensional (2D) materials has emerged as a promising strategy to tailor their electronic, magnetic, and adsorption properties, enabling promising applications in energy storage and spintronics devices. In this work, spin-polarized density functional theory (DFT) calculations were employed to investigate the ground state properties and hydrogen (H2) storage of interstitially X = As and Sb atom doped B6P6 (B6P6X) graphenylene monolayers. The resulting B6P6X (X = As, Sb) monolayers exhibit very good mechanical, dynamical, and thermal stabilities with antiferromagnetic (AFM) ground states. Electronic structure calculations reveal AFM semiconducting behavior for both monolayers, with indirect/direct band gaps of 0.71/0.60 eV (PBE) and 2.19/2.14 eV (HSE06) for B6P6As/B6P6Sb, respectively. All B6P6X monolayers exhibit an in-plane easy magnetization axis. The obtained Berezinskii-Kosterlitz–Thouless transition (BKT) temperature value of B6P6Sb monolayer is 268.74 K. Furthermore, the H2 storage capabilities of these B6P6X monolayers were examined. We find that B6P6As and B6P6Sb monolayers can each adsorb up to 48H2 molecules with an average adsorption energy (Ea) of -0.14 eV/H2. The corresponding H2 storage gravimetric capacities are 6.91 wt% for B6P6As@48H2 and 6.10 wt% for B6P6As@48H2, surpassing the U.S. Department of Energy’s 2025 target of 5.50 wt%. These findings highlighting the potential of B6P6X (X = As, Sb) monolayers for AFM spintronics and H2 storage applications.

Tuning Sb Atoms on Cu‐Based Catalysts for Electrochemical Conversion of CO2 to Syngas

The electrochemical CO2RR into syngas provides an attractive way to produce raw materials for synthesizing various value‐added chemicals. However, a wide range of tunable syngas ratio of CO/H2 is hard to achieve during the electrochemical CO2 conversion process. Herein, we propose a facile electrodeposition method for the preparation of Sb modified Cu‐based catalyst with a high activity for the ratio‐tunable production of syngas. The Cu10Sb1 catalyst reaches a high FE of 71% for CO at a potential of ‐1.09 V vs. RHE with the tunable CO/H2 ratio of syngas from ~0.6 to ~7.8 at the applied potentials from ‐0.78 V to ‐1.09 V. Theoretical calculations reveal the tuning effect of Sb atoms on Cu‐based catalyst for the electrochemical conversion of CO2 to syngas, in which the formation of CO on Sb modified Cu‐based catalyst possesses low energy barrier in potential‐limiting steps during CO2RR. Meanwhile, the robust charge interaction between COOH* species and the surface of Sb modified Cu‐based catalyst enhances the activity of COOH* species, thus improving FE and current for conversion into syngas products. This work brings a new strategy for the synthesis of low‐cost syngas catalyst and the tuning effect of metal atom on Cu‐based catalyst for CO2RR.

Synthesis of Sb688-: Crafting a Homoatomic Antimony Nanotorus.

Pure-element cyclic molecules have garnered extensive attention owing to their intriguing structures and promising applications. Among these, carbon-based cyclic molecules such as cyclo[n]carbon (Cn, n = 10-26) and carbon nanotori have ignited significant interest in both experimental and theoretical investigations. However, systematic investigations of analogous cyclic counterparts of heavier main-group elements are limited, with only a few known by theoretical studies. Furthermore, these corresponding cyclic structures lack synthetic examples in the condensed phase, primarily attributed to their high reactivity resulting from lone electron pairs and the absence of electronic delocalization, which typically aids in stabilizing the structure. In this work, we introduce the pioneering synthesis of a pure antimony-based inorganic nanotorus, denoted as Sb688-, facilitated by the incorporation of C60 for oxidation by utilizing wet-chemistry methodologies. The unique nanotorus structure was meticulously examined via single-crystalline X-ray diffraction, unveiling its composition of 68 antimony atoms and forming a tubular structure with approximate dimensions of 18.5 × 18.4 Å2 in a square shape. Theoretical calculations further revealed that the nanotorus structure, characterized by 16 delocalized electrons distributed across eight 3c-2e σ bonds, effectively saturated the eight two-coordinated Sb atoms within the cluster. This study unveils an innovative approach to synthesizing cyclic compounds solely from pure elements, departing from traditional methods dependent on chemical vapor deposition or surface synthesis, and heralds a profound paradigm shift in physical science.

Epitaxial Growth of Large-Scale α-Phase Antimonene.

Two-dimensional materials composed of elements from the 15th group of the periodic table remain largely unexplored. The primary challenge in advancing this research is the lack of large-scale layers that would facilitate extensive studies using laterally averaging techniques and enable functionalization for the fabrication of novel electronic, optoelectronic, and spintronic devices. In this report, we present a method for synthesizing large-scale antimonene layers, on the order of cm2. By employing molecular beam epitaxy, we successfully grow a monolayer film of α-phase antimonene on a W(110) surface passivated with a single-atom-thick layer of Sb atoms. The formation of α phase antimonene is confirmed through scanning tunneling microscopy and low-energy electron diffraction measurements. The isolated nature of the α-phase is further evidenced in the electronic structure, with linearly dispersed bands observed through angle-resolved photoelectron spectroscopy and supported by ab initio calculations.

Study of the fundamental physical characteristics of the Zintl phase K2BaCdSb2

The structural, elastic, thermodynamic, electronic, and thermoelectric characteristics of K2BaCdSb2 were investigated utilizing ab initio methods. The structural, elastic, and thermodynamic properties were calculated using the pseudopotential plane wave approach with the GGA-PBEsol exchange-correlation functional. The computed equilibrium structural characteristics closely match the available data. The anticipated elastic constants reveal that K2BaCdSb2 is mechanically stable, brittle, and exhibits significant elastic anisotropy. The full potential linearized augmented plane wave approach with the Tran-Blaha modified Becke-Johnson potential was used to determine the electronic structure of K2BaCdSb2.It is found that K2BaCdSb2 is a semiconductor with a Γ-Γ type direct bandgap of 0.85 eV. Bonding analysis shows the bond between Cd and Sb atoms within the [CdSb2]4− polyanion is of covalent nature and that between the K/Ba atom and the [CdSb2]4− polyanion is of ionic character. The thermoelectric characteristics of K2BaCdSb2 were analyzed at a temperature of 500 K for of charge-carrier concentrations from 1 × 1018 to 3 × 1020 cm−3.When the concentration of holes is 1.0 × 1020 cm−3, The power factor reaches a value of 17 × 1010 W m−1 K−2.s−1 for a hole concentration of 1.0 × 1020 cm−3. For the p-doped K2BaCdSb2 with a concentration of 1.0 × 1018cm−3, the electronic figure of merit is 0.95.

Long-Chain Molecular Crystals Antimony(III) Alkanethiolates Sb(SCnH2n+1)3 (n ≥ 12): Synthesis, Crystal and Electronic Structures, and Supramolecular Self-Assembly via Secondary Interactions.

Currently, there is not much success in solving the molecular and crystal structures of long-chain metal alkanethiolate complexes [M(SCnH2n+1)m] at the atomic level. Taking Sb(SC16H33)3 (1) as an example, we herein disclose the structural characteristics of long-chain trivalent antimony(III) alkanethiolates Sb(SCnH2n+1)3 (n ≥ 12) by single-crystal X-ray crystallography. Specifically, the Sb atom is three-coordinated by alkanethiolate ligands and a slightly distorted triangular pyramid SbS3 core is formed owing to the unique intramolecular stereochemistry of three alkyl chains, namely, two of them almost parallel aligning and the third chain extending alone around the SbS3 core. We further determine the conformation, spatial orientation and packing density of alkyl chains in 1 along with a comparison to those in other long-chain crystalline systems, and reveal the roles of intermolecular van der Waals and Sb···S secondary interactions in molecular self-assembly, which enables 1 to be a layer-structured molecular crystal with a monoclinic P21/c unit cell. The band structures and the atomic orbital contributions to the valence band maximum and conduction band minimum for 1 have also been evaluated by DFT calculations and rationally correlated with its optical absorption property. This study will help understand and discover new structures and structure-property relations of long-chain chemical systems.

Template Selection Strategy for Synthesis of One-Dimensional CrSbSe3 Ferromagnetic Semiconductor Nanoribbons.

CrSbSe3─the only experimentally validated one-dimensional (1D) ferromagnetic semiconductor─has recently attracted significant attention. However, all reported synthesis methods for CrSbSe3 nanocrystals are based on top-down methods. Here we report a template selection strategy for the bottom-up synthesis of CrSbSe3 nanoribbons. This strategy relies on comparing the formation energies of potential binary templates to the ternary target product. It enables us to select Sb2Se3 with the highest formation energy, along with its 1D crystal structure, as the template instead of Cr2Se3 with the lowest formation energy, thereby facilitating the transformation from Sb2Se3 to CrSbSe3 by replacing half of the Sb atoms in Sb2Se3 with Cr atoms. The as-prepared CrSbSe3 nanoribbons exhibit a length of approximately 5 μm, a width ranging from 80 to 120 nm, and a thickness of about 5 nm. The single CrSbSe3 nanoribbon presents typical semiconductor behavior and ferromagnetism, confirming the intrinsic ferromagnetism in the 1D CrSbSe3 semiconductor.

Modulation of monolayer SnSe2 optoelectronic properties by applied electric field and atomic doping

Based on the first principles, we have calculated the influence of the applied electric field and doped X (X = N, P, As, Sb) atoms on the optoelectronic properties and phonon dispersion of the monolayer 2D material SnSe2. The calculation results show that intrinsic SnSe2 is a semiconductor with a band gap value of 0.884 eV. The doping of X atoms improves the energy band tunability of the monolayer SnSe2 system and becomes more stable. The N-doped SnSe2 system has the most stable structure and the best doping performance. When the electric field strength of 0.3 V/Å is applied on the surface of the N-doped system, the band gap of the system increases. The energy gap gradually decreases when the electric field strength continues to increase from 0.3 V/Å to 0.9 V/Å. At an applied electric field strength of 0.9 V/Å, the system changes from semiconductor to metallic properties. As far as the optical properties are concerned, the applied electric field increases the static refractive index of the system, the imaginary part of the photoconductivity increases, the energy loss function decreases, and the light absorption performance improves. The applied electric field successfully enhanced the optical properties of the SnSe2 system. The applied electric field strength of 0.9 V/Å doped N system has the best optical properties. This provides a new way to explore the optoelectronic devices based on the SnSe2 doped system.

Analogous Chelation to Boost Utilization of Sb in Sb Nanoparticles and N-doped Carbon Composites for Enhancing Potassium Storage.

Antimony (Sb) is an attractive anode material for potassium-ion batteries (PIBs), but it suffers from aggregation during the charging-discharging process, thus causing embedded active sites and collapsed structure. The analogous chelation refers to the reaction in which the central nanoparticle is linked to the matrix through multiple coordination bonds to form a stable composite. This strategy can inhibit aggregation and maintain the nanosized structure of Sb, thus activating the utilization of Sb active sites and structural stability. Given the special position of nitrogen (N) in the periodic table of elements and the strong bond energy of Sb-N, the N element can serve as an intermediate to connect Sb nanoparticles and an intrinsic N-doped carbon network via strong Sb-N-C/Sb-N═C covalent bonds using analogous chelation. Herein, a hybrid material of Sb@CTF-NC is fabricated via analogous chelation. The Sb atoms exposed on the surface of Sb nanoparticles are used to chelate with the N-doped carbon for high-performance PIBs. The mechanism underwent ex situ characterizations. The calculation of density functional theory reveals that the increase of adsorption energy and reduction of the K+ diffusion barrier accelerate the electrochemical reaction kinetics.

Turning copper into an efficient and stable CO evolution catalyst beyond noble metals

Using renewable electricity to convert CO2 into CO offers a sustainable route to produce a versatile intermediate to synthesize various chemicals and fuels. For economic CO2-to-CO conversion at scale, however, there exists a trade-off between selectivity and activity, necessitating the delicate design of efficient catalysts to hit the sweet spot. We demonstrate here that copper co-alloyed with isolated antimony and palladium atoms can efficiently activate and convert CO2 molecules into CO. This trimetallic single-atom alloy catalyst (Cu92Sb5Pd3) achieves an outstanding CO selectivity of 100% (±1.5%) at −402 mA cm−2 and a high activity up to −1 A cm−2 in a neutral electrolyte, surpassing numerous state-of-the-art noble metal catalysts. Moreover, it exhibits long-term stability over 528 h at −100 mA cm−2 with an FECO above 95%. Operando spectroscopy and theoretical simulation provide explicit evidence for the charge redistribution between Sb/Pd additions and Cu base, demonstrating that Sb and Pd single atoms synergistically shift the electronic structure of Cu for CO production and suppress hydrogen evolution. Additionally, the collaborative interactions enhance the overall stability of the catalyst. These results showcase that Sb/Pd-doped Cu can steadily carry out efficient CO2 electrolysis under mild conditions, challenging the monopoly of noble metals in large-scale CO2-to-CO conversion.

A Sterically Accessible Monomeric Stibine Oxide Activates Organotetrel(IV) Halides, Including C-F and Si-F Bonds.

Phosphine oxides and arsine oxides are common laboratory reagents with diverse applications that stem from the chemistry exhibited by these monomeric species. Stibine oxides are, in contrast, generally dimeric or oligomeric species because of the reactivity-quenching self-association of the highly polarized stiboryl (Sb=O/Sb+-O-) group. We recently isolated Dipp3SbO (Dipp = 2,6-diisopropylphenyl), the first example of a kinetically stabilized monomeric stibine oxide, which exists as a bench-stable solid and bears an unperturbed stiboryl group. Herein, we report the isolation of Mes3SbO (Mes = mesityl), in which the less bulky substituents maintain the monomeric nature of the compound but unlock access to a wider range of reactivity at the unperturbed stiboryl group relative to Dipp3SbO. Mes3SbO was found to be a potent Lewis base in the formation of adducts with the main-group Lewis acids PbMe3Cl and SnMe3Cl. The accessible Lewis acidity at the Sb atom results in a change in the reactivity with GeMe3Cl, SiMe3Cl, and CPh3Cl. With these species, Mes3SbO formally adds the E-Cl (E = Ge, Si, C) bond across the unsaturated stiboryl group to form a 5-coordinate stiborane. The biphilicity of Mes3SbO is sufficiently potent to activate even the C-F and Si-F bonds of C(p-MeOPh)3F and SiEt3F, respectively. These results mark a significant contribution to an increasingly rich literature on the reactivity of polar, unsaturated main-group motifs. Furthermore, these results highlight the utility of a kinetic stabilization approach to access unusual bonding motifs with unquenched reactivity that can be leveraged for small-molecule activation.

Crystallization behavior and structural characteristics of Cr-doped Sb70Se30 thin films for phase change memory

In this study, we prepare Cr-doped Sb70Se30 (SS) thin films via the magnetron sputtering. The influence of Cr doping on the crystallization behavior and structure characteristics of the SS thin films is systematically studied using a combination of experimental analyzes and theoretical calculations. The results reveal that compared with SS thin films, Cr-doped SS thin films exhibit higher crystallization temperature, better data retention capability, larger crystallization activation energy, and reduced resistance drift coefficient. In addition, the incorporation of Cr effectively suppresses grain growth in the SS thin films and refines the grain size. The electrical transport properties of the Cr-doped SS thin films are analyzed using a Hall system. Both X-ray photoelectron spectroscopy and first-principles calculations indicate that Cr is more prone to occupy Sb atoms and form stronger Cr–Se bonds, consequently enhancing the stability of the SS thin films. Raman spectroscopy confirms that the introduction of Cr leads to a decrease in bond length and an increase in bond energy. Moreover, the Cr-doped SS thin film exhibits minimal volume fluctuations and a smoother surface morphology, resulting in enhanced interface performance and reliability. Taken together, these results indicate that the introduction of Cr is an effective strategy for optimizing the properties and modifying the structures of SS phase-change materials.

High-performance quantum anomalous Hall effect in monolayer Ti2Sb2KRb and Ti2Bi2NaK

Quantum anomalous Hall (QAH) insulators are an ideal platform for developing topological electronic devices, but their low observation temperature limits the applications. In this study, based on first-principles calculations, monolayer Ti2Sb2KRb and Ti2Bi2NaK are demonstrated to be QAH insulators with topological gaps 43 and 57 meV, respectively. Their Chern numbers are calculated to be C=−2. The study of electronic structures indicates that the ferromagnetic topological property is induced by the energy band inversion of dxy and dx2−y2 orbitals for Ti atoms near the Dirac cone. Both monolayer Ti2Sb2KRb and Ti2Bi2NaK exhibit a perpendicular magnetic anisotropy, and their Curie temperatures are estimated to be 480 and 478 K, respectively. The ferromagnetic coupling is induced by the small crystal-field splitting energy caused by Sb and Bi atom's large radius. Our study suggests that monolayer Ti2Sb2KRb and Ti2Bi2NaK are promising candidates for room temperature QAH insulators.

Structural, optical, and electrical analysis of tailoring Bi2-xSbxTe3 thin films

Bismuth antimony telluride (Bi2-xSbxTe3) thin films were synthesized using chemical bath deposition (CBD) with various amounts of antimony. The structural, morphological, and optical properties of Bi2-xSbxTe3 thin films have been scrutinized using X-ray diffraction (XRD), field-emission scanning electron microscopy (FESEM), UV-Vis spectrophotometry. A higher amount of Sb contents can be observed the Sb0.405Te0.595, BiTe, and Bi4Te3 phases consisted in the pattern. Meanwhile, the energy band gaps are tuned in the range of 2.95 to 3.30 eV. Finally, measurement of resistance with various temperatures for activation energy (EAC) estimation was performed. The highest EAC value was equal to 0.654 eV for 0.8 g SbCl3 as a precursor of Sb atom incorporated in the Bi2Te3 lattice.

Structural evolution and thermoelectric performance in (GeTe)m(Sb2Te3)n compounds

Exploring the relationship between crystal structure and thermoelectric performance is a pivotal topic in the thermoelectric field. In this study, we have comprehensively investigated the correlation between the structural evolution of (GeTe)m(Sb2Te3)n pseudo-binary system and the thermoelectric properties. The proportion of van der Waals bonds increases with the rising Sb2Te3 content, resulting in an increase in the anisotropy of the electrical conductivity and a decrease in the average sound velocity. Additionally, the cation sites in the crystal lattice of these compounds exhibit a mixed occupancy of Ge/Sb atoms, although the cation sites adjacent to the van der Waals gaps are predominantly occupied by Sb atoms. The ultra-low lattice thermal conductivity of the GST124 and GST147 compounds is mainly attributed to the high concentration of van der Waals bonds and enhanced phonon scattering arising from Ge/Sb mixed cation occupancy and high density of defect structures. The high electrical conductivity combined with the low lattice thermal conductivity enables GST124 and GST147 compounds to achieve a maximum ZT value of 0.56 and 0.57, respectively. Higher thermoelectric performance can be achieved through optimization of the microstructure as well as the carrier concentration.

Effects of working pressure during magnetron sputtering on thermoelectric performance of flexible p-type Bi0.5Sb1.5Te3 thin films

The influence of argon working pressure during magnetron sputtering on thermoelectric properties has been investigated on p-type Bi0.5Sb1.5Te3 flexible films deposited at various working pressures in the range from 2 to 5 Pa. The microstructure and orientations, atomic compositions, and carrier concentration could be regulated by adjusting the working pressure, due to the size-dependent inhibition of the deposition of the sputtered Bi, Sb, and Te atoms from argon ions. Profiting from the occurrence of the (006) orientation, the nearest stoichiometric ratio, the highest carrier concentration and mobility, and the quantum confinement effect, the film deposited at 4 Pa displays the maximum power factor of 1095 μW m−1 K−2 at 360 K. These results suggest that the electrical transport properties of the sputtered flexible thermoelectric thin films can be synergistically optimized by selecting an appropriate working pressure.

The competition between charge density wave and superconductivity in the kagome metal CsV3(Sb1-xPbx)5 single crystals

Kagome metal AV3Sb5 (A = K, Rb, Cs) has garnered considerable attention for its abundant exotic quantum phenomena and the special competitive relationship between charge density wave (CDW) and superconductivity (SC). In this work we explore the unconventional coupling between charge density wave and superconductivity by means of the substitutional doping of Pb atoms with Sb atoms. Microscopic characterization and performance tests provide valuable phase diagram information for CsV3(Sb1-xPbx)5. Upon Pb doping, a pronounced competition between the charge density wave transition temperature TCDW and the superconducting temperature Tc was observed. Analysis of changes in Debye temperature ΘD and lattice constant, it is shown that Pb doping affects atomic bonding and may strengthen the coupling between adjacent kagome layers to some extent. Furthermore, the small angular shift of the diffraction peak and increased full width at half maximum (FWHM) indicate that the doping causes crystal defects and distorts the crystal structure, which will change the charge density in the local area and may affect the superconductivity. This result further reveals a close correlation between the superconductivity of the system and the electronic structure of the kagome plane in the CsV3Sb5 system. Overall, our results suggest that the observed competition arises from the complex interplay of multiple factors.

Electronic structure and optical properties of nitrogen-doped antimonene under biaxial strain: first-principles study.

In this thesis, the role of N atom doping and biaxial strain in modulating the electronic structure and optical properties of antimonene has been deeply investigated using a first-principles approach based on density-functional theory. The results show that N doping significantly reduces the band gap of antimonene and introduces new electronic states, thus affecting its electronic structure. In terms of optical properties, N doping reduces the static permittivity of antimonene and alters its absorption, reflection, and energy loss properties. In addition, biaxial strain further enhanced the modulation effect of these properties. This study not only provides theoretical support for the application of antimonene in the field of high-performance two-dimensional electronic and optoelectronic devices, but also reveals strain and doping as an effective means to modulate the physical properties of two-dimensional materials. For the calculations, we used the DFT-based CASTEP software package for the simulation of the electronic structure. In order to more accurately characterize the weak interactions between two-dimensional materials, we specifically introduced the Van der Waals dispersion correction. We have chosen the Perdew-Burke-Ernzerhof (PBE) exchange-correlation generalization under the generalized gradient approximation (GGA) and combined it with the Van der Waals correction term in order to fully consider the electronic structure of antimonene. For the calculation parameter settings, we set the truncation energy to 400 eV to ensure the accuracy of the calculation. Meanwhile, we adopt a 6 × 6 × 1 k-point grid for Brillouin zone sampling to obtain more accurate energy band structure and density of states information. For the convergence settings, the convergence criteria for both the system energy and the interaction force between atoms were set to 1 × 10-5 eV and 0.01 eV/Å, respectively. We selected a 3 × 3 × 1 supercell model with 18 Sb atoms. A vacuum thickness of 18 Å was established in the Z direction, which is sufficient to avoid interactions between the two atomic layers above and below the periodic structure.

Modifying Roles of CuSbSe2 in Realizing High Thermoelectric Performance of GeTe

AbstractThermoelectric materials are widely researched for their energy conversion capabilities in the fields of power generation and refrigeration. And a superior thermoelectric conversion efficiency requires an excellent power factor and low thermal conductivity. Herein, a remarkable thermoelectric figure of merit（ZT） ∼ 2.6 at 673 K is realized in GeTe with 20% addition of CuSbSe2. Multiple synergistic effects of CuSbSe2 alloying collectively contribute to the excellent thermoelectric performance in GeTe. CuSbSe2 alloying effectively tunes ultrahigh carrier density of GeTe to the optimum. The introduction of Cu, Sb, and Se atoms create numerous point defects that scatter high‐frequency phonons. Additionally, surplus CuSbSe2 facilitates the formation of copper‐selenium phases, which embed at grain boundaries and generate interfaces after sintering. Combining the planar defects evolved from Ge vacancies, multi‐dimension defects effectively scatter multiple frequency phonons. An extraordinarily low lattice thermal conductivity of 0.3 Wm−1 K−1 at 673 K is obtained, approaching the theoretical estimation predicted by Cahill model. Eventually, the peak conversion efficiency of 7.4% is obtained in segmented device with ΔT of 419 K. The commingled effects of CuSbSe2 in GeTe further open up an elitist route to designing high‐performance materials.