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Carbon quantum dots (CQDs) are promising carbonaceous nanomaterials fortuitously discovered in 2004. CQDs are the rising stars in the nanotechnology ensemble because of their unique properties and widespread applications in sensing, imaging, medicine, catalysis, and optoelectronics. CQDs are notable for their excellent solubility and effective luminescence and, as a result, they are also known as carbon nanolights. Many strategies are used for the efficient and economical preparation of CQDs; however, CQDs prepared from waste or green sustainable methods have greater requirements due to their safety and ease of synthesis. Sustainable chemical strategies for CQDs have been developed, emphasizing green synthetic methodologies based on 'top-down' and 'bottom-up' approaches. This review summarizes many such studies relevant to the development of sustainable methods for photoluminescent CQDs. Furthermore, we have emphasized recent advances in CQDs' photoluminescence applications in chemical and biological fields. Finally, a brief overview of synthetic processes using the green source and their associated applications are tabulated, providing a clear understanding of the new optoelectronic materials.
Assuntos
Pontos Quânticos , Pontos Quânticos/química , Carbono/química , Luminescência , CatáliseRESUMO
We report on magnetization M(H), dc and ac magnetic susceptibility χ(T), specific heat C_{m}(T) and muon spin relaxation (µSR) measurements of the Kitaev honeycomb iridate Cu_{2}IrO_{3} with quenched disorder. In spite of the chemical disorders, we find no indication of spin glass down to 260 mK from the C_{m}(T) and µSR data. Furthermore, a persistent spin dynamics observed by the zero-field muon spin relaxation evidences an absence of static magnetism. The remarkable observation is a scaling relation of χ[H,T] and M[H,T] in H/T with the scaling exponent α=0.26-0.28, expected from bond randomness. However, C_{m}[H,T]/T disobeys the predicted universal scaling law, pointing towards the presence of additional low-lying excitations on the background of bond-disordered spin liquid. Our results signify a many-faceted impact of quenched disorder in a Kitaev spin system due to its peculiar bond character.
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Thermoelectric energy harvesting-the transformation of waste heat into useful electricity-is of great interest for energy sustainability. The main obstacle is the low thermoelectric efficiency of materials for converting heat to electricity, quantified by the thermoelectric figure of merit, ZT. The best available n-type materials for use in mid-temperature (500-900 K) thermoelectric generators have a relatively low ZT of 1 or less, and so there is much interest in finding avenues for increasing this figure of merit. Here we report a binary crystalline n-type material, In(4)Se(3-delta), which achieves the ZT value of 1.48 at 705 K-very high for a bulk material. Using high-resolution transmission electron microscopy, electron diffraction, and first-principles calculations, we demonstrate that this material supports a charge density wave instability which is responsible for the large anisotropy observed in the electric and thermal transport. The high ZT value is the result of the high Seebeck coefficient and the low thermal conductivity in the plane of the charge density wave. Our results suggest a new direction in the search for high-performance thermoelectric materials, exploiting intrinsic nanostructural bulk properties induced by charge density waves.
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This study reports the synthesis of type-I Ba8CuNi2.5Ga10Si33.5 clathrate as a single crystal by the flux method and physical properties investigations such as structural, chemical, magnetic, and thermal properties. Structural refinements indicate Ba atoms are situated at 2a and 6d positions with mixed occupancy across framework sites. Raman spectroscopy assessed host-guest interactions, while the compound's morphology and composition were investigated by the scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS), and X-ray photoelectron spectroscopy (XPS) analyses. Magnetic properties revealed ferromagnetic interactions characterized by a positive Weiss constant and weak ferromagnetic hysteresis. The compound's metallic nature is evidenced by increased resistivity with temperature. The Sommerfeld coefficient, estimated at 12.59 mJ mol-1 K-2 from heat capacity data, alongside a pronounced peak around 15 K in the Cp/T3 vs T plot, suggests an Einstein contribution in heat capacity.
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We investigated the magnetocaloric and electrical transport properties of the Eu8CuNi2.5Si42.5 clathrate compound, synthesized by an arc melting and annealing method. X-ray photoemission spectroscopy revealed a mixed valence state of Eu2+ and Eu3+. The low-field and low-temperature magnetic measurements indicated a multiple magnetic transition, from ferromagnetic near 35 K to antiferromagnetic at 25 K. Increasing the magnetic field led to the broadening of antiferromagnetic peaks and a final ferromagnetic state under high magnetic fields, indicative of spin reorientation. The transition from a ferromagnetic to an antiferromagnetic state was further corroborated by specific heat measurements. We noted spontaneous magnetization at low temperatures via magnetic hysteresis and Arrott plot analysis. The coexistence of an antiferromagnetic ground state (attributed to the Eu2+ ions) and ferromagnetic clusters (associated with the Ni2+ ions) was supported by spontaneous magnetization at low temperatures in the antiferromagnetic state. The magnetocaloric analyses revealed a high spin entropy change over a broad temperature range for Eu8CuNi2.5Si42.5, which implies its potential as a robust low-temperature magnetocaloric material, distinguished by its high refrigerant capacity.
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We study the thermoelectric properties of a p-type Bi0.4Sb1.6Te3.4 (BST) composite with Ag nanoparticle-decorated TiO2 microparticles (US-Ag/TiO2). The dispersion of US-Ag/TiO2 particles, synthesized by an ultrasonication (US) method, into the matrix effectively decreases lattice and bipolar thermal conductivity, attributed to the scattering centers formed at nano and micro scales. The electron backscattering diffraction (EBSD) measurements revealed smaller grain sizes within the BST composite when paired with the US-Ag/TiO2 particle dispersion. These reduced grain sizes, alongside nanoparticle-decorated microparticles dispersed throughout the matrix, scatter phonons effectively from long- to short-wavelength phonons and subsequently decrease lattice thermal conductivity. While the power factors of the composites are reduced, significant suppression of lattice and bipolar thermal conductivity has led to an increase in the maximum zT value (1.4 at 325 K) for a 0.9 wt % US-Ag/TiO2 particle dispersion within the BST matrix. This particle dispersion in the BST composite consistently demonstrates a high zT value across an extensive temperature spectrum, leading to an exceptionally high average zTavg value (1.38 up to 400 K), which is superior to the other values from reported BST composites. Thus, this research indicates that the dispersion of nanoparticle-decorated microparticles within a thermoelectric material matrix can significantly improve thermoelectric performance, which has promising implications for practical applications in thermoelectric cooling and sustainable and economical energy harvesting technologies.
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Magnetic anisotropy strongly influences the performance of the magnetocaloric effect. We investigated the magnetocaloric properties of the NdAlGe single crystal with I41md structure. The temperature-dependent magnetization revealed significant anisotropic properties; stable antiferromagnetic transition at TN = 6 K for H//a and meta-magnetic spin reorientation at low temperature (T ≤ 5 K) within an intermediate field (H = 2 T) for H//c. During the metamagnetic spin reorientation, the abrupt change of the magnetic entropy leads to a significant magnetocaloric effect with negative magnetic entropy change (∆SM) by -13.80 J kg-1 K-1 at TC = 5.5 K for H = 5 T along the H//c axis. In addition, the antiferromagnetic state for H//a shows the inverse magnetocaloric effect(I-MCE) by positive entropy change ∆SM = 2.64 J kg-1 K-1 at TN = 6 K for H = 5 T. This giant MCE accompanied by the metamagnetic transition resulted in a significantly large relative cooling power (158 J/kg at H = 5 T) for H//c. The giant MCE and I-MCE can be applied to the rotational magnetocaloric effect (R-MCE) depending on the crystal orientations. NdAlGe exhibits rotational entropy change ∆Sc-a = -12.85 J kg-1 K at Tpeak = 7.5 K, H = 5 T. With comparison to conventional MCE materials, NdAlGe is suggested as promising candidate of R-MCE, which is a novel type of magnetic refrigeration system.
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We investigated the colors of graphene and graphene-oxide multilayers that were deposited on various dielectric layers. In particular, the effects of the material thickness, the types of dielectric layers, and the existence of a back silicon substrate were analyzed. The colors of graphene-oxide layers on a SiO2/Si substrate were found to periodically change as the material thickness increased. However, the colors of graphene layers on the same substrate became saturated without a similar periodic change. The calculated colors corresponding to the material thicknesses were verified by optical microscopy and profilometry. We believe that these results demonstrate the possibility of utilizing color as a simple tool for detecting and estimating the thicknesses of graphene and graphene-oxide multilayers.
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The present study develops a general framework for weak antilocalization (WAL) in a three-dimensional (3D) system, which can be applied for a consistent description of longitudinal resistivity [Formula: see text] and Hall resistivity [Formula: see text] over a wide temperature (T) range. Compared to the previous approach Vu et al. (Phys Rev B 100:125162, 2019), which assumes infinite phase coherence length (lÏ) and a zero spin-orbit scattering length (lSO), the present framework is more general, covering high T and the intermediate spin-orbit coupling strength. Based on the new approach, the [Formula: see text] and [Formula: see text] of the Dirac semimetal Bi0.97Sb0.03 was analyzed over a wide T range from 1.7 to 300 K. The present framework not only explains the main features of the experimental data but also enables one to estimate lÏ and lSO at different temperatures. The lÏ has a power-law T dependence at high T and saturates at low T. In contrast, the lSO shows negligible T dependence. Because of the different T dependence, a crossover occurs from the lSO-dominant low-T to the lÏ-dominant high-T regions. Accordingly, the hallmark features of weak antilocalization (WAL) in [Formula: see text] and [Formula: see text] are gradually suppressed across the crossover with increasing T. The present theory describes both low-T and high-T regions successfully, which is impossible in the previous approximate approach. This work offers insights for understanding quantum electrical transport phenomena and their underlying physics, particularly when multiple WAL length scales are competing.
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High-entropy alloy (HEA) superconductors-a new class of functional materials-can be utilized stably under extreme conditions, such as in space environments, owing to their high mechanical hardness and excellent irradiation tolerance. However, the feasibility of practical applications of HEA superconductors has not yet been demonstrated because the critical current density (Jc) for HEA superconductors has not yet been adequately characterized. Here, we report the fabrication of high-quality superconducting (SC) thin films of Ta-Nb-Hf-Zr-Ti HEAs via a pulsed laser deposition. The thin films exhibit a large Jc of >1 MA cm-2 at 4.2 K and are therefore favorable for SC devices as well as large-scale applications. In addition, they show extremely robust superconductivity to irradiation-induced disorder controlled by the dose of Kr-ion irradiation. The superconductivity of the HEA films is more than 1000 times more resistant to displacement damage than that of other promising superconductors with technological applications, such as MgB2, Nb3Sn, Fe-based superconductors, and high-Tc cuprate superconductors. These results demonstrate that HEA superconductors have considerable potential for use under extreme conditions, such as in aerospace applications, nuclear fusion reactors, and high-field SC magnets.
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We investigated the thermoelectric properties of the Pb0.75Sn0.25Se and Pb0.79Sn0.25Se1-xClx (x = 0.0, 0.2, 0.3, 0.5, 1.0, 2.0 mol.%) compounds, synthesized by hot-press sintering. The electrical transport properties showed that low concentration doping of Cl (below 0.3 mol.%) in the Pb-excess (Pb,Sn)Se samples increased the carrier concentration and the Hall mobility by the increase of carriers' mean free path. The effective mass of the carrier was also enhanced from the measurements of the Seebeck coefficient. The enhanced effective masses of the carrier by the Cl-doping can be understood by the enhanced electron-phonon interaction, caused by the crystalline mirror symmetry breaking. The significantly decreased lattice thermal conductivities showed that the crystalline mirror symmetry breaking decreased the lattice thermal conductivity of the Pb-excess (Pb,Sn)Se. By the Cl-doping and the Pb-excess's synergistic effect, which can suppress the bipolar effect, the zT values of x = 0.2 and 0.3 mol.% reached 0.8 at 773 K. Therefore, we suggest that Pb-excess and the crystalline mirror symmetry breaking by Cl-doping are effective for high thermoelectric performance in the (Pb,Sn)Se.
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Bismuth-Telluride-based compounds are unique materials for thermoelectric cooling applications. Because Bi2Te3 is a narrow gap semiconductor, the bipolar diffusion effect is a critical issue to enhance thermoelectric performance. Here, we report the significant reduction of thermal conductivity by decreasing lattice and bipolar thermal conductivity in extrinsic phase mixing of MgO and VO2 nanoparticles in Bi0.5Sb1.5Te3 (BST) bulk matrix. When we separate the thermal conductivity by electronic κel, lattice κlat, and bipolar κbi thermal conductivities, all the contributions in thermal conductivities are decreased with increasing the concentration of oxide particle distribution, indicating the effective phonon scattering with an asymmetric scattering of carriers. The reduction of thermal conductivity affects the improvement of the ZT values. Even though significant carrier filtering effect is not observed in the oxide bulk composites due to micro-meter size agglomeration of particles, the interface between oxide and bulk matrix scatters carriers giving rise to the increase of the Seebeck coefficient and electrical resistivity. Therefore, we suggest the extrinsic phase mixing of nanoparticles decreases lattice and bipolar thermal conductivity, resulting in the enhancement of thermoelectric performance over a wide temperature range.
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We investigated the anisotropic thermoelectric properties of the Bi2Te2.85Se0.15Ix (x = 0.0, 0.1, 0.3, 0.5 mol.%) compounds, synthesized by ball-milling and hot-press sintering. The electrical conductivities of the Bi2Te2.85Se0.15Ix were significantly improved by the increase of carrier concentration. The dominant electronic scattering mechanism was changed from the mixed (T ≤ 400 K) and ionization scattering (T ≥ 420 K) for pristine compound (x = 0.0) to the acoustic phonon scattering by the iodine doping. The Hall mobility was also enhanced with the increasing carrier concentration. The enhancement of Hall mobility was caused by the increase of the mean free path of the carrier from 10.8 to 17.7 nm by iodine doping, which was attributed to the reduction of point defects without the meaningful change of bandgap energy. From the electron diffraction patterns, a lattice distortion was observed in the iodine doped compounds. The modulation vector due to lattice distortion increased with increasing iodine concentration, indicating the shorter range lattice distortion in real space for the higher iodine concentration. The bipolar thermal conductivity was suppressed, and the effective masses were increased by iodine doping. It suggests that the iodine doping minimizes the ionization scattering giving rise to the suppression of the bipolar diffusion effect, due to the prohibition of the BiTe1 antisite defect, and induces the lattice distortion which decreases lattice thermal conductivity, resulting in the enhancement of thermoelectric performance.
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Developing inexpensive and rapid fabrication methods for high efficiency thermoelectric alloys is a crucial challenge for the thermoelectric industry, especially for energy conversion applications. Here, we fabricated large amounts of p-type Cu0.07Bi0.5Sb1.5Te3 alloys, using water atomization to control its microstructure and improve thermoelectric performance by optimizing its initial powder size. All the water atomized powders were sieved with different aperture sizes, of 32-75 µm, 75-125 µm, 125-200 µm, and <200 µm, and subsequently consolidated using hot pressing at 490 °C. The grain sizes were found to increase with increasing powder particle size, which also increased carrier mobility due to improved carrier transport. The maximum electrical conductivity of 1457.33 Ω-1 cm-1 was obtained for the 125-200 µm samples due to their large grain sizes and subsequent high mobility. The Seebeck coefficient slightly increased with decreasing particle size due to scattering of carriers at fine grain boundaries. The higher power factor values of 4.20, 4.22 × 10-3 W/mk2 were, respectively, obtained for large powder specimens, such as 125-200 µm and 75-125 µm, due to their higher electrical conductivity. In addition, thermal conductivity increased with increasing particle size due to the improvement in carriers and phonons transport. The 75-125 µm powder specimen exhibited a relatively high thermoelectric figure of merit, ZT of 1.257 due to this higher electric conductivity.
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One promising approach to improving thermoelectric energy conversion is to use nanostructured interfaces that enhance Seebeck coefficient while reducing thermal conductivity. Here, we synthesized Au-Cu2Se core-shell nanoparticles with different shell thicknesses by controlling the precursor concentration in solution. The Au-Cu2Se core-shell nanoparticles are about 37-53 nm in size, and the cores of the nanostructures are composed of Au nanoparticles with sizes of â¼11 nm. The effect of shell thickness on the thermoelectric properties of core-shell nanocomposites is investigated after sintering the core-shell nanoparticles into pellets using the spark plasma sintering (SPS) technique. The power factor was optimized by the synergetic effect of the improvement of Seebeck coefficient by energy filtering in the Au/Cu2Se interface and the effective tuning of carrier concentration by Ohmic contact in the interface. The lattice thermal conductivity of core-shell nanocomposites is reduced by coherent phonon scattering, which is caused by the wavelike interference of phonons due to the phase shift in the core-shell interface. The highest ZT value of 0.61 is obtained at 723 K for Au-Cu2Se core-shell nanocomposite with a shell thickness of 21 nm, which is higher than that of pure Cu2Se nanocomposite or a mixture of Au and Cu2Se particles.
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We investigate the thermoelectric properties of (CuI)0.003Bi2Te2.7Se0.3/Mo (Mo: 0.0, 0.9, 1.3, 1.8, 3.1, and 4.3 vol %) composites, which were synthesized by extrinsic phase mixing with hot press sintering. From X-ray diffraction (XRD) and energy-dispersive X-ray spectroscopy (EDX) measurements, we confirm that micro-sized Mo particles are dispersed homogeneously in the (CuI)0.003Bi2Te2.7Se0.3 matrix without doping. While the electrical resistivity of Mo-dispersed (CuI)0.003Bi2Te2.7Se0.3 composites is not changed significantly, the Seebeck coefficient is significantly increased. Because the work function (5.3 eV) of the (CuI)0.003Bi2Te2.7Se0.3 compounds, measured by ultraviolet photoelectron spectroscopy (UPS), is larger than that of Mo particles (4.95 eV), we expect the potential barrier near the interfaces between the BTS matrix and Mo particles. The band bending effect and potential barrier can give rise to the low-energy carrier filtering. For a low concentration dispersion of Mo particles (<2 vol %), a decrease of Hall carrier concentration, an increase of Hall mobility, a decrease of effective mass, and an increase of Seebeck coefficient also support the formation of low-energy carrier filtering. The Mo dispersion does not affect the decrease in the lattice thermal conductivity but enhances the power factor significantly, leading to the high ZT value above 1.0 at room temperature, which is a high level in n-type thermoelectric room-temperature applications.
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Bi2Te3-based compounds have long been studied as thermoelectric materials in cooling applications near room temperature. Here, we investigated the thermoelectric properties of CuI-doped Bi2Te2.1Se0.9 compounds. The Cu/I codoping induces the lattice distortion partially in the matrix. We report that the charge density wave caused by the local lattice distortion affects the electrical and thermal transport properties. From the high-temperature specific heat, we found a first-order phase transitions near 490 and 575 K for CuI-doped compounds (CuI)xBi2Te2.1Se0.9 (x = 0.3 and 0.6%), respectively. It is not a structural phase transition, confirming from the high-temperature X-ray diffraction. The temperature-dependent electrical resistivity shows a typical behavior of charge density wave transition, which is consistent with the temperature-dependent Seebeck coefficient and thermal conductivity. The transmission electron microscopy and electron diffraction show a local lattice distortion, driven by the charge density wave transition. The charge density wave formation in the Bi2Te3-based compounds are exceptional because of the possibility of coexistence of charge density wave and topological surface states. From the Kubo formula and Boltzmann transport calculations, the formation of charge density wave enhances the power factor. The lattice modulation and charge density wave decrease lattice thermal conductivity, resulting in the enhancement of thermoelectric performance simultaneously in CuI-doped samples. Consequently, an enhancement of thermoelectric performance ZT over 1.0 is achieved at 448 K in the (CuI)0.003Bi2Te2.1Se0.9 sample. The enhancement of ZT at high temperature gives rise to a superior average ZTavg (1.0) value than those of previously reported ones.
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Bi2Te3-based compounds have received attention as thermoelectric materials for room-temperature cooling and waste heat recovery applications. With potential application prospects, quaternary compounds of Bi2Te3-Bi2Se3-Bi2S3 composites can be used for mid-temperature power generation under 500 °C. Herein, we investigated the thermoelectric properties of (CuI) y (Bi2Te3)0.95-x (Bi2Se3) x (Bi2S3)0.05 (x = 0.05, 0.2; y = 0.0, 0.003) compounds. Through X-ray diffraction and transmission electron microscopy, we confirmed that the lattice disorder in (Bi2Te3)0.95-x (Bi2Se3) x (Bi2S3)0.05 (x = 0.2) was due to multiple element substitutions. Disorder carrier scattering induced the localized nature of electrical resistivity, as confirmed by variable range hopping at low temperature. The temperature-dependent Seebeck coefficient of (Bi2Te3)0.95-x (Bi2Se3) x (Bi2S3)0.05 showed a carrier-type change from p- to n-type behaviour in the intermediate temperature range (525 K for x = 0.05 and 360 K for x = 0.2). Even though strong carrier localization increased electrical resistivity, resulting in degradation of the power factor and thermoelectric performance, when the chemical potential was increased to the conduction band minimum through CuI co-doping into the (CuI)0.003(Bi2Te3)0.95-x (Bi2Se3) x (Bi2S3)0.05 (x = 0.05, 0.2) compounds, the carriers were delocalized and showed n-type behaviour in the Seebeck coefficient. The temperature-dependent thermal conductivity shows the suppression of bipolar conduction behaviour. The simultaneous effect on carrier optimization through chemical potential tuning and lattice disorder caused a high ZT value of 0.85 at 523 K for CuI-doped (Bi2Te3)0.75(Bi2Se3)0.2(Bi2S3)0.05, which was comparatively high for n-type thermoelectric materials in the mid-temperature range.
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Considerable efforts have been devoted to enhancing thermoelectric performance, by employing phonon scattering from nanostructural architecture, and material design using phonon-glass and electron-crystal concepts. The nanostructural approach helps to lower thermal conductivity but has limited effect on the power factor. Here, we demonstrate selective charge Anderson localization as a route to maximize the Seebeck coefficient while simultaneously preserving high electrical conductivity and lowering the lattice thermal conductivity. We confirm the viability of interface potential modification in an n-type Bi-doped PbTe/Ag2Te nanocomposite and the resulting enhancement in thermoelectric figure-of-merit ZT. The introduction of random potentials via Ag2Te nanoparticle distribution using extrinsic phase mixing was determined using scanning tunneling spectroscopy measurements. When the Ag2Te undergoes a structural phase transition ( T > 420 K) from monoclinic ß-Ag2Te to cubic α-Ag2Te, the band gap in the α-Ag2Te increases due to the p -d hybridization. This results in a decrease in the potential barrier height, which gives rise to partial delocalization of the electrons, while wave packets of the holes are still in a localized state. Using this strategic approach, we achieved an exceptionally high thermoelectric figure-of-merit in n-type PbTe materials, a ZT greater than 2.0, suitable for waste heat power generation.
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Topological insulators generally share commonalities with good thermoelectric (TE) materials because of their narrow band gaps and heavy constituent elements. Here, we propose that a topological crystalline insulator (TCI) could exhibit a high TE performance by breaking its crystalline symmetry and tuning the chemical potential by elemental doping. As a candidate material, we investigate the TE properties of the Cl-doped TCI Pb0.7Sn0.3Se. The infrared absorption spectra reveal that the band gap is increased from 0.055 eV for Pb0.7Sn0.3Se to 0.075 eV for Pb0.7Sn0.3Se0.99Cl0.01, confirming that the Cl doping can break the crystalline mirror symmetry of a TCI Pb0.7Sn0.3Se and thereby enlarge its bulk electronic band gap. The topological band inversion is confirmed by the extended X-ray absorption fine structure spectroscopy, which shows that the TCI state is weakened in a chlorine x = 0.05-doped compound. The small gap opening and partial linear band dispersion with massless and massive bands may have a high power factor (PF) for high electrical conductivity with an enhancement of the Seebeck coefficient. As a result, Pb0.7Sn0.3Se0.99Cl0.01 shows a considerably enhanced ZT of 0.64 at 823 K, which is about 1200% enhancement in ZT compared with that of the undoped Pb0.7Sn0.3Se. This work demonstrates that the optimal n-type Cl doping tunes the chemical potential together with breaking the state of the TCI, suppresses the bipolar conduction at high temperatures, and thereby enables the Seebeck coefficient to increase up to 823 K, resulting in a significantly enhanced PF at high temperatures. In addition, the bipolar contribution to thermal conductivity is effectively suppressed for the Cl-doped samples of Pb0.7Sn0.3Se1- xCl x ( x ≥ 0.01). We propose that breaking the crystalline mirror symmetry in TCIs could be a new research direction for exploring high-performance TE materials.