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学者姓名：罗中箴
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Abstract ：
Low-grade heat (below 373 Kelvins) is abundant and ubiquitous, yet the lack of cost-effective recovery technologies frequently impedes its effective utilization. The advent of thermogalvanic hydrogel thermocells has garnered significant attention due to their high thermopower, inherent flexibility, low cost, and scalability. Thermogalvanic hydrogels have significantly enhanced their thermoelectric performance, resulting in the development of functional materials that exhibit flexibility, stretchability, self-healing, and frost resistance. However, there are substantial challenges in developing multifunctional thermogalvanic hydrogels that combine high power density and efficiency with practical applicability. This review discusses the synthesis of the novel redox couple, improving the performance of electrolytes to increase thermopower, creating electrodes with extensive surface areas for better current density and flexibility, and optimizing thermocell structure design to improve performance further. This comprehensive review aims to propel progress toward higher performance levels and broader applications of thermogalvanic hydrogel thermocells.
Keyword ：
energy output energy output thermocell thermocell thermogalvanic effect thermogalvanic effect Thermogalvanic hydrogel Thermogalvanic hydrogel thermopower thermopower
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| GB/T 7714 | Liu, Wei , Fang, Yi , Lyu, Xiaolin et al. Construction and application of thermogalvanic hydrogels [J]. | SOFT SCIENCE , 2024 , 4 (4) . |
| MLA | Liu, Wei et al. "Construction and application of thermogalvanic hydrogels" . | SOFT SCIENCE 4 . 4 (2024) . |
| APA | Liu, Wei , Fang, Yi , Lyu, Xiaolin , Peng, Xiangfang , Luo, Zhong-Zhen , Zou, Zhigang . Construction and application of thermogalvanic hydrogels . | SOFT SCIENCE , 2024 , 4 (4) . |
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The Pb4Sb12-xBi8+xSe34 (x = 0, 1, 2, 3, 4, and 5) crystals belong to pavonite homologues composed of thick NaCl- and thin GeS-type slabs which crystallize in the C2/m space group. Pb4Sb12-xBi8+xSe34 compounds exhibit n-type semiconductor transport behavior and demonstrate excellent thermodynamic stability. These intrinsic compounds have high carrier concentrations of similar to 2.18 x 10(19) to 4.47 x 10(20) cm(-3), leading to high electrical conductivities. The two-band electronic structure results in a high Seebeck coefficient. Taking Pb4Sb9Bi11Se34 as an example, it has a remarkable Seebeck coefficient of -149.1 mu V K-1 and high electrical conductivity of similar to 118 S cm(-1). It is comparable with other pavonite at 723 K. On the other hand, due to mixed occupancies of cation sites and complex crystal structure, the Pb4Sb9Bi11Se34 features ultralow lattice thermal conductivity of similar to 0.25 W m(-1) K-1 at 723 K. The high figure of merit, ZT, of 0.48 for Pb4Sb9Bi11Se34 is obtained at 723 K.
Keyword ：
crystal structure crystal structure pavonite pavonite Pb4Sb12-x Bi8+x Se34 Pb4Sb12-x Bi8+x Se34 thermoelectric thermoelectric ultralow thermalconductivity ultralow thermalconductivity
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| GB/T 7714 | Yang, Ruizhi , Li, Xia , Ming, Hongwei et al. Crystal Structure and Thermoelectric Properties of Pavonite Homologous Pb4Sb12-x Bi8+x Se34 [J]. | ACS APPLIED ENERGY MATERIALS , 2024 , 7 (11) : 4942-4949 . |
| MLA | Yang, Ruizhi et al. "Crystal Structure and Thermoelectric Properties of Pavonite Homologous Pb4Sb12-x Bi8+x Se34" . | ACS APPLIED ENERGY MATERIALS 7 . 11 (2024) : 4942-4949 . |
| APA | Yang, Ruizhi , Li, Xia , Ming, Hongwei , Guo, Weiping , Chen, Zixuan , Cui, Hong-Hua et al. Crystal Structure and Thermoelectric Properties of Pavonite Homologous Pb4Sb12-x Bi8+x Se34 . | ACS APPLIED ENERGY MATERIALS , 2024 , 7 (11) , 4942-4949 . |
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Although orthorhombic GeSe is predicted to have an ultrahigh figure of merit, ZT approximate to 2.5, up to now, the highest experimental value is approximate to 0.2 due to the low carrier concentration (n(H) approximate to 10(18) cm(-3)). Improving symmetry is an effective approach for enhancing the ZT of GeSe-based materials. With Te-alloying, Ge4Se3Te displays the two-dimensional hexagonal structure and high n(H) approximate to 1.23 x 10(21) cm(-3). Interestingly, Ge4Se3Te transformed from the hexagonal into the rhombohedral phase with only approximate to 2% I-V-VI2-alloying (I = Li, Na, K, Cu, Ag; V = Sb, Bi; VI = Se, Te). According to the calculated results of Ge0.82Ag0.09Bi0.09Se0.614Te0.386 single-crystal grown via AgBiTe2-alloying, it exhibits a higher valley degeneracy than the hexagonal Ge4Se3Te. For instance, AgBiTe2-alloying induces a strong band convergence and band inversion effect, resulting in a significantly enhanced Seebeck coefficient and power factor with a similar n(H) from 17 mu V K-1 and 0.63 mu W cm(-1) K-2 for pristine Ge4Se3Te to 124 mu V K-1 and 5.97 mu W cm(-1) K-2 for 12%AgBiTe2-alloyed sample, respectively. Moreover, the sharply reduced phonon velocity, nano-domain wall structure, and strong anharmonicity lead to low lattice thermal conductivity. As a result, a record-high average ZT approximate to 0.95 over 323-773 K with an excellent ZT approximate to 1.30 is achieved at 723 K.
Keyword ：
Ge4Se3Te Ge4Se3Te multi-band convergence multi-band convergence nano-domain wall structure nano-domain wall structure symmetry manipulation symmetry manipulation thermoelectricity thermoelectricity
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| GB/T 7714 | Guo, Mingjie , Cui, Hong-Hua , Guo, Weiping et al. Achieving Superior Thermoelectric Performance in Ge4Se3Te via Symmetry Manipulation with I-V-VI2 Alloying [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (18) . |
| MLA | Guo, Mingjie et al. "Achieving Superior Thermoelectric Performance in Ge4Se3Te via Symmetry Manipulation with I-V-VI2 Alloying" . | ADVANCED FUNCTIONAL MATERIALS 34 . 18 (2024) . |
| APA | Guo, Mingjie , Cui, Hong-Hua , Guo, Weiping , Chen, Zixuan , Ming, Hongwei , Luo, Zhong-Zhen et al. Achieving Superior Thermoelectric Performance in Ge4Se3Te via Symmetry Manipulation with I-V-VI2 Alloying . | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (18) . |
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Five new semiconductors Pb5Sb12+xBi6-xSe32 (x = 0, 1, 2, 3, and 4) have been synthesized for the first time, which adopt pavonite-type structure and crystallize in monoclinic C2/m space group. The crystal structure is composed of two different types of polyhedral slabs. Slab-I is a galena-like structure motif that forms with [MSe6] (M = Pb, Sb, and Bi) octahedra and slab-II contains one octahedral [MSe6] block and paired squared pyramids [MSe5]. Pb5Sb12+xBi6-xSe32 exhibits n-type semiconductor behaviors and the remarkable Seebeck coefficient from -64.1 mu V K-1 for x = 0 sample to -242 mu V K-1 for x = 4 sample at 300 K. Moreover, the Pb5Sb12Bi6Se32 has the highest carrier concentration of 1.35 x 10(20) cm(-3) in pavonite-type materials. The complex compositions, mixed occupancies of the cations, and quasi-two-dimensional structure lead to the low lattice thermal conductivity (kappa(lat)) less than 0.48 W m(-1) K-1 from 300 to 723 K, at which Pb5Sb16Bi2Se32 especially shows the ultralow value of 0.25 W m(-1) K-1. As a result, the thermoelectric figure of merit, ZT similar to 0.34 at 723 K, is obtained for the intrinsic Pb5Sb12Bi6Se32.
Keyword ：
Mixed occupancies Mixed occupancies Pavonite-type structure Pavonite-type structure Pb5Sb12Bi6Se32 Pb5Sb12Bi6Se32 Semiconductors Semiconductors Thermoelectric Thermoelectric Ultralow thermal conductivity Ultralow thermal conductivity
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| GB/T 7714 | Yang, Ruizhi , Li, Xia , Guo, Weiping et al. New thermoelectric semiconductors Pb5Sb12+xBi6-xSe32 with ultralow thermal conductivity [J]. | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2024 , 43 (3) . |
| MLA | Yang, Ruizhi et al. "New thermoelectric semiconductors Pb5Sb12+xBi6-xSe32 with ultralow thermal conductivity" . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY 43 . 3 (2024) . |
| APA | Yang, Ruizhi , Li, Xia , Guo, Weiping , Chen, Zixuan , Ming, Hongwei , Luo, Zhong-Zhen et al. New thermoelectric semiconductors Pb5Sb12+xBi6-xSe32 with ultralow thermal conductivity . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2024 , 43 (3) . |
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Improving polarizability is an important strategy for designing high-performance mid-infrared (mid-IR) nonlinear optical (NLO) materials. The substitution of equivalent or aliovalent atoms can manipulate the polarizability by adjusting the symmetry of the polyhedron. Herein, the Li+ and Cd2+ are introduced into the Cu3PS4 as the equivalent and aliovalent dopants for the Cu site. As a result, Li+ can significantly improve the bandgap (E-g) of LixCu3-xPS4 from 2.38 to 2.88 eV, leading to a higher laser-induced damage threshold (LIDT) of 4.9 times than AgGaS2 (AGS) with a comparable second harmonic generation (SHG) response of AGS (26-45 mu m). Interestingly, Cd2+ can improve the SHG response and enlarge the E-g simultaneously. As a result, Cd0.4Cu2.2PS4 has a large SHG response of 10 x AGS at 2050 nm (26-45 mu m) and a LIDT of 2.6 x AGS. Theoretical calculations reveal that lattice vacancies induced by Cd2+ significantly boost polarizability compared to LixCu3-xPS4 with no vacancy, leading to a strong NLO response.
Keyword ：
aliovalent substitution aliovalent substitution lattice vacancies lattice vacancies Mid-IR NLO Mid-IR NLO polarizability polarizability SHG response SHG response
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| GB/T 7714 | Guo, Weiping , Fu, Yudi , Cui, Hong-Hua et al. Vacancy-Induced Extraordinary Second Harmonic Generation Response for Diamond-Like Cu3PS4 [J]. | ADVANCED OPTICAL MATERIALS , 2024 , 12 (18) . |
| MLA | Guo, Weiping et al. "Vacancy-Induced Extraordinary Second Harmonic Generation Response for Diamond-Like Cu3PS4" . | ADVANCED OPTICAL MATERIALS 12 . 18 (2024) . |
| APA | Guo, Weiping , Fu, Yudi , Cui, Hong-Hua , Li, Lingyun , Yu, Yan , Luo, Zhong-Zhen et al. Vacancy-Induced Extraordinary Second Harmonic Generation Response for Diamond-Like Cu3PS4 . | ADVANCED OPTICAL MATERIALS , 2024 , 12 (18) . |
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Time-resolved multiterahertz (THz) spectroscopy is used to observe an ultrafast, nonthermal electronic phase change in SnSe driven by interband photoexcitation with 1.55 eV pump photons. The transient THz photoconductivity spectrum is found to be Lorentzian-like, indicating charge localization and phase segregation. The rise of photoconductivity is bimodal in nature, with both a fast and slow component due to excitation into multiple bands and subsequent intervalley scattering. The THz conductivity magnitude, dynamics, and spectra show a drastic change in character at a critical excitation fluence of approximately 6 mJ/cm2 due to a photoinduced phase segregation and a macroscopic collapse of the band gap.
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| GB/T 7714 | Dringoli, Benjamin J. , Sutton, Mark , Luo, Zhongzhen et al. Ultrafast Photoinduced Phase Change in SnSe [J]. | PHYSICAL REVIEW LETTERS , 2024 , 132 (14) . |
| MLA | Dringoli, Benjamin J. et al. "Ultrafast Photoinduced Phase Change in SnSe" . | PHYSICAL REVIEW LETTERS 132 . 14 (2024) . |
| APA | Dringoli, Benjamin J. , Sutton, Mark , Luo, Zhongzhen , Kanatzidis, Mercouri G. , Cooke, David G. . Ultrafast Photoinduced Phase Change in SnSe . | PHYSICAL REVIEW LETTERS , 2024 , 132 (14) . |
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Hydrogel thermocells possess great potential in the energy conversion field as they directly absorb waste heat from the environment to drive redox reactions for continuous electricity generation. However, achieving high toughness and good elasticity simultaneously in hydrogel thermocells remains a challenge because of the inherent contradiction of energy dissipation mechanisms, severely limiting their practical applications and lifespan. To address this, a skin-like hydrogel network with a highly dense interwoven network is developed to construct hydrogel thermocells with good elasticity and high toughness. The dense network structure can effectively disperse the stress and hinder crack propagation, thus breaking the contradiction between high toughness and good elasticity. The thermocell realizes a toughness of 460 J m−2 while reaching an elastic limit strain of 350 %, far exceeding the elasticity of previous stretchable hydrogel thermocells. Meanwhile, it exhibits ultra-low hysteresis and excellent fatigue resistance under tensile and compressive cyclic loads. Moreover, the thermocell can work stably over long periods, enabling stable voltage output even under compression, bending, and stretching. In addition, the thermocell can power the LED lamp and calculator, and can also be connected in series to form large arrays, thus rendering it an ideal power source for wearable devices. © 2024 Elsevier B.V.
Keyword ：
Ductile fracture Ductile fracture Elasticity Elasticity Electric loads Electric loads Energy dissipation Energy dissipation Energy utilization Energy utilization Hydrogels Hydrogels Redox reactions Redox reactions Waste heat Waste heat Wearable technology Wearable technology
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| GB/T 7714 | Lyu, Xiaolin , Lin, Ziqing , Huang, Chunzhi et al. Tough and elastic hydrogel thermocells for heat energy utilization [J]. | Chemical Engineering Journal , 2024 , 493 . |
| MLA | Lyu, Xiaolin et al. "Tough and elastic hydrogel thermocells for heat energy utilization" . | Chemical Engineering Journal 493 (2024) . |
| APA | Lyu, Xiaolin , Lin, Ziqing , Huang, Chunzhi , Zhang, Xinyue , Lu, Yang , Luo, Zhong-Zhen et al. Tough and elastic hydrogel thermocells for heat energy utilization . | Chemical Engineering Journal , 2024 , 493 . |
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PbS is an attractive thermoelectric material with low cost, high thermostability, and large abundance in the Earth's crust. However, its largest energy difference between the light and heavy valence bands (ΔEv) leads to a huge challenge in achieving valence band convergence (VBC), resulting in the lowest power factor (PF) compared to PbSe and PbTe. This low PF impedes the output power density of thermoelectric devices. In this work, the Ag dopant can reduce ΔEv from 0.34 eV to 0.20 eV, achieving VBC in p-type PbS for the first time, significantly improving the Seebeck coefficient. Additionally, Pb0.98Ag0.02S exhibits semiconductor-like electrical conductivity caused by the grain boundaries scattering below 473 K. With coarse-graining, the mobility improves substantially from 4.6 cm2 V−1 s−1 to 241 cm2 V−1 s−1 at room temperature. Consequently, the PF of Pb0.98Ag0.02S increases from 0.3 μW cm−1 K−2 to 12.2 μW cm−1 K−2 with the figure of merit ZT value rising from 0.0027 to 0.10 at 300 K. More importantly, Pb0.98Ag0.02S crystal maintains a high PF from 300 K to 823 K, giving a record-high average PF of 13.0 μW cm−1 K−2 and an increased ZT. This work certifies Ag as an effective p-type dopant for weakening electron transport coupling for PbS-based thermoelectric materials. © 2024 Elsevier B.V.
Keyword ：
Coarse-graining Coarse-graining Power factor Power factor P-type PbS P-type PbS Thermoelectric Thermoelectric Valence band convergence Valence band convergence
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| GB/T 7714 | Wu, M. , Cui, H.-H. , Chen, Z. et al. Realization of valence band convergence for high thermoelectric performance p-type PbS [J]. | Chemical Engineering Journal , 2024 , 494 . |
| MLA | Wu, M. et al. "Realization of valence band convergence for high thermoelectric performance p-type PbS" . | Chemical Engineering Journal 494 (2024) . |
| APA | Wu, M. , Cui, H.-H. , Chen, Z. , Zhou, J. , Ming, H. , Luo, Z.-Z. et al. Realization of valence band convergence for high thermoelectric performance p-type PbS . | Chemical Engineering Journal , 2024 , 494 . |
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Low-cost copper (Cu)-based electrocatalysts have been widely established with the special capability of generating C2+ products from the CO2 reduction reaction (CO2RR). However, efficient formate production has been rarely achieved due to the instant reduction of most reported Cu-based catalysts upon CO2RR, and the derived metallic Cu compromises the C1 selectivity. Herein, we demonstrate that the incorporation of alkali metal ions is intrinsically effective for stabilizing the Cu(I)-S bonds by forming ternary copper sulfides (M-Cu(I)-S, M = Na, K, and Rb). The strengthened Cu-S bonds can be well preserved in M-Cu(I)-S during the CO2RR, contributing to the protonation effect and thus highly efficient production of formate. Moreover, the M-Cu(I)-S catalysts also exhibit enhanced electrical conductivity relative to that of Cu2S, favorably promoting the reaction kinetics. Accordingly, the RbCu7S4 as a representative catalyst achieves a Faradaic efficiency of 90.4 ± 1.3% for formate at only −0.7 V versus reversible hydrogen electrode (VRHE), with a high partial current density of 272.1 mA cm-2 and stable operation over 72 h. This study could provide a different series of Cu-based electrocatalysts for efficient formate production on an industrial scale from the CO2RR. © 2024 American Chemical Society.
Keyword ：
alkali metal alkali metal CO2 reduction CO2 reduction Cu-based catalyst Cu-based catalyst Cu−S bond Cu−S bond formate formate
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| GB/T 7714 | Cui, X. , Wu, M. , Hou, G. et al. Alkali Metal Ions Stabilizing Copper(I)-Sulfur Bonds for Efficient Formate Production from Electrochemical CO2 Reduction [J]. | ACS Catalysis , 2024 , 14 (15) : 11857-11864 . |
| MLA | Cui, X. et al. "Alkali Metal Ions Stabilizing Copper(I)-Sulfur Bonds for Efficient Formate Production from Electrochemical CO2 Reduction" . | ACS Catalysis 14 . 15 (2024) : 11857-11864 . |
| APA | Cui, X. , Wu, M. , Hou, G. , Li, Y. , Wang, Y. , Huang, J. et al. Alkali Metal Ions Stabilizing Copper(I)-Sulfur Bonds for Efficient Formate Production from Electrochemical CO2 Reduction . | ACS Catalysis , 2024 , 14 (15) , 11857-11864 . |
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Band convergence is considered a net benefit to thermoelectric performance as it decouples the density of states effective mass (md & lowast;$m_{\mathrm{d}}<^>{\mathrm{*}}$) and carrier mobility (mu) by increasing valley degeneracy. Unlike conventional methods that typically prioritize md & lowast;$m_{\mathrm{d}}<^>{\mathrm{*}}$ at the expense of mu, this study theoretically demonstrates an unconventional band convergence strategy to enhance both md & lowast;$m_{\mathrm{d}}<^>{\mathrm{*}}$ and mu in SnTe under pressure. Density functional theory calculations reveal that increasing pressure from 0 to 5 GPa moves the Sigma-band of SnTe upward, reducing the energy offset between L- and Sigma-band from 0.35 to 0.2 eV while preserving the light band feature of the L-band. Consequently, a high power factor (PF) of 119.2 mu W cm-1 K-2 at 300 K is achieved for p-type SnTe under 5 GPa. Chemical pressure also induces conduction band convergence, significantly enhancing the PF of n-type SnTe. Additionally, the interplay between pressure-induced phonon modes leads to a moderate increase in lattice thermal conductivity of SnTe below 3 GPa, which combined with the significantly enhanced PF, contributes to a large enhancement in ZT. Consequently, predicted ZT values of 2.12 at 650 K and 2.55 at 850 K are obtained for p- and n-type SnTe, respectively, showcasing substantial performance enhancements.
Keyword ：
band convergence band convergence chemical pressure chemical pressure fermi velocity fermi velocity phonon scattering phonon scattering SnTe SnTe
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| GB/T 7714 | Ming, Hongwei , Luo, Zhong-Zhen , Zou, Zhigang . Chemical Pressure-Induced Unconventional Band Convergence Leads to High Thermoelectric Performance in SnTe [J]. | ADVANCED SCIENCE , 2024 , 12 (1) . |
| MLA | Ming, Hongwei et al. "Chemical Pressure-Induced Unconventional Band Convergence Leads to High Thermoelectric Performance in SnTe" . | ADVANCED SCIENCE 12 . 1 (2024) . |
| APA | Ming, Hongwei , Luo, Zhong-Zhen , Zou, Zhigang . Chemical Pressure-Induced Unconventional Band Convergence Leads to High Thermoelectric Performance in SnTe . | ADVANCED SCIENCE , 2024 , 12 (1) . |
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