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Pressure Distinguishes the Dual Emissions in Pseudohalide 2D Ruddlesden-Popper Perovskite Cs_(2)Pb(SCN)_(2)Br2

CCS Chemistry 2024年第7期6卷 1748-1756页

作者： Songhao Guo Yuhong Mao Congcong Chen Yao Zhang Guoxiang Zhao Kejun Bu Qingyang Hu Haiming Zhu Guifu Zou Wenge Yang Lingling Mao Xujie Lü Center for High Pressure Science and Technology Advanced Research(hpstar) Shanghai Department of Chemistry Southern University of Science and TechnologyShenzhen Department of Chemistry Zhejiang UniversityHangzhou College of Energy Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu ProvinceSoochow UniversitySuzhou

Two-dimensional(2D)Ruddlesden-Popper(RP)halide perovskites with diverse structures and properties have drawn increasing attention due to their promising optoelectronic ***,a new all-inorganic Cs_(2)Pb(SCN)_(2)Br_(2) has been reported that opens up new potential for the development of 2D RP ***,recent reports of unusual dual emissions and two-edge absorption in Cs_(2)Pb(SCN)_(2)Br_(2) have generated intense debate about its origin and remains ***,by combining continuous pressure tuning with in situ diagnostics,we have unambiguously revealed the underlying mechanisms that the 2D Cs_(2)Pb(SCN)_(2)Br_(2) exhibits an intrinsic blue emission at 2.66 eV and an absorption edge close to the emission *** the gradually formed CsPbBr3 is responsible for the green emission at 2.33 eV with the absorption shoulder at 2.41 ***,by fitting the temperature-dependent intensity of the intrinsic blue emission,we have determined the corrected value of exciton binding energy for 2D Cs_(2)Pb(SCN)_(2)Br_(2) to be 90 ***,an emission enhancement of 2.5 times is achieved in Cs_(2)Pb(SCN)_(2)Br_(2) under a mild pressure within 0.8 GPa,caused by the pressuresuppressed exciton-phonon *** work not only elucidates the origin of the dual emissions and two-edge absorption in Cs_(2)Pb(SCN)_(2)Br_(2),but it also provides a potential means to regulate and optimize the optoelectronic properties of 2D perovskites.

关键词： two-dimensional perovskite dual emissions two-edge absorption high pressure in situ characterization enhanced photoluminescence

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类施主效应调控与高择优取向织构提升n型Bi_(2)(Te,Se)_(3)材料热电性能

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Science Bulletin 2024年第11期69卷 1728-1737页

作者：李奕辰白树林文熠赵哲王磊刘世博郑俊卿王斯琦刘姗高德政刘东锐朱英才曹茜高翔谢鸿耀赵立东 School of Materials Science and Engineering Beihang UniversityBeijing 100191China Tianmushan Laboratory Hangzhou 311115China Huabei Cooling Device Co.LTD. Langfang 065400China Center for High Pressure Science and Technology Advanced Research(hpstar) Beijing 100094China

Thermoelectric materials have a wide range of application because they can be directly used in refrigeration and power generation. And the Bi_(2)Te_(3) stand out because of its excellent thermoelectric performance and are used in commercial thermoelectric devices. However, n-type Bi_(2)Te_(3) has seriously hindered the development of Bi_(2)Te_(3)-based thermoelectric devices due to its weak mechanical properties and inferior thermoelectric performance. Therefore, it is urgent to develop a high-performance n-type Bi_(2)Te_(3) polycrystalline. In this work, we employed interstitial Cu and the hot deformation process to optimize the thermoelectric properties of Bi_(2)Te_(2.7)Se_(0.3), and a high-performance thermoelectric module was fabricated based on this material. Our combined theoretical and experimental effort indicates that the interstitial Cu reduce the defect density in the matrix and suppresses the donor-like effect, leading to a lattice plainification effect in the material. In addition, the two-step hot deformation process significantly improves the preferred orientation of the material and boosts the mobility. As a result, a maximum ZT of 1.27 at 373 K and a remarkable high ZT_(ave) of 1.22 across the temperature range of 300–425 K are obtained. The thermoelectric generator(TEG, 7-pair) and thermoelectric cooling(TEC, 127-pair) modules were fabricated with our n-type textured Cu_(0.01)Bi_(2)Te_(2.7)Se_(0.3) coupled with commercial p-type Bi_(2)Te_(3). The TEC module demonstrates superior cooling efficiency compared with the commercial Bi_(2)Te_(3) device, achieving a ΔT of 65 and 83.4 K when the hot end temperature at 300 and 350 K, respectively. In addition, the TEG module attains an impressive conversion efficiency of 6.5% at a ΔT of 225 K, which is almost the highest value among the reported Bi_(2)Te_(3)-based TEG modules.

关键词： Bi_(2)Te_(3) Texture engineering TEC TEG Donor-like effect

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Structurally Flexible 2D Spacer for Suppressing the Electron-Phonon Coupling Induced Non-Radiative Decay in Perovskite Solar Cells

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Nano-Micro Letters 2024年第9期16卷 325-340页

作者： Ruikun Cao Kexuan Sun Chang Liu Yuhong Mao Wei Guo Ping Ouyang Yuanyuan Meng Ruijia Tian Lisha Xie Xujie Lü Ziyi Ge Zhejiang Provincial Engineering Research Center of Energy Optoelectronic Materials and Devices Ningbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo 315201People’s Republic of China School of Materials Science and Chemical Engineering Ningbo UniversityNingbo 315211People’s Republic of China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049People’s Republic of China Center for High Pressure Science and Technology Advanced Research(hpstar) Shanghai 201203People’s Republic of China

This study presents experimental evidence of the dependence of non-radiative recombination processes on the electron-phonon coupling of perovskite in perovskite solar cells(PSCs).Via A-site cation engineering,a weaker electron-phonon coupling in perovskite has been achieved by introducing the structurally soft cyclohexane methylamine(CMA^(+))cation,which could serve as a damper to alleviate the mechanical stress caused by lattice oscillations,compared to the rigid phenethyl methylamine(PEA^(+))*** demonstrates a significantly lower non-radiative recombination rate,even though the two types of bulky cations have similar chemical passivation effects on perovskite,which might be explained by the suppressed carrier capture process and improved lattice geometry *** resulting PSCs achieve an exceptional power conversion efficiency(PCE)of 25.5%with a record-high opencircuit voltage(V_(OC))of 1.20 V for narrow bandgap perovskite(FAPbI_(3)).The established correlations between electron-phonon coupling and non-radiative decay provide design and screening criteria for more effective passivators for highly efficient PSCs approaching the Shockley-Queisser limit.

关键词： Electron-phonon coupling A-site cation engineering Non-radiative recombination

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Enhancing reversibility of LiNi_(0.5)Mn_(1.5)O_(4)by regulating surface oxygen deficiency

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Carbon Energy 2023年第11期5卷 81-89页

作者： Dandan Wang Cong Gao Xuefeng Zhou Shang Peng Mingxue Tang Yonggang Wang Lujun Huang Wenge Yang Xiang Gao Center for High Pressure Science and Technology Advanced Research(hpstar) BeijingChina School of Materials Science and Engineering Harbin Institute of TechnologyHarbinChina

Oxygen deficiency has crucial effects on the crystal structure and electrochemical performance of spinel oxide lithium electrode materials such as LiNi_(0.5)Mn_(1.5)O_(4)(LNMO)*** particular,the oxygen stoichiometry on the crystal surface differs from that on the crystal interior in *** detection of local oxygen loss in LNMO and its correlation with the crystal structure and the cycling stability of LNMO remain *** this study,the effect of oxygen deficiency in LNMO controlled by sintering temperature on the surface crystal structure and electrochemical performance of LNMO is comprehensively *** high concentration of oxygen vacancies segregates at the surface regions of LNMO forming a thin rock‐salt and/or deficient spinel surface *** atomic‐level surface structure reconstruction was demonstrated by annular dark‐field and annular brightfield *** the synthesis of LNMO,the higher sintering temperature results in higher crystallinity but the higher oxygen deficiency in *** high crystallinity of LNMO would increase the thermal stability of LNMO cathodes while the high content of oxygen deficiency would decrease the surface structural stability of ***,the LNMO sintered at a medium temperature of 850°C achieved the best capacity *** results suggest a competitive function mechanism between oxygen stoichiometry and the crystallinity of LNMO on the cycling performance of LNMO.

关键词： electrochemical performance LiNi_(0.5)Mn_(1.5)O_(4) lithium‐ion battery oxygen vacancies surface reconstruction

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Yi-Gang Xu: the Earth's deep interior holds the key to habitability

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National Science Review 2021年第4期8卷 35-38页

作者： Jin Liu Ho-Kwang Mao the Center for High Pressure Science and Technology Advanced Research (hpstar) hpstar

The deep Earth is the engine of whole Earth systems and plays a key role in surface evolution and geological hazards. Scientists have been deciphering the internal processes that shape our habitable planet, especially since the formulation of plate tectonics theory. To date, how the deep Earth works remains mysterious. At the end of 2020,

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Pressure-driven symmetry breaking and electron disproportionation of the trigonal Nb_(3)cluster in Nb_(3)Cl_(8)

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Science China(Physics,Mechanics & Astronomy) 2022年第7期65卷 153-158页

作者： Zimin Jiang Dequan Jiang Yiming Wang Chen Li Ke Liu Ting Wen Fuyang Liu Zhengyang Zhou Yonggang Wang Center for High Pressure Science and Technology Advanced Research(hpstar) Beijing 100094China Shanghai Institute of Ceramics Chinese Academy of SciencesShanghai 201899China

Symmetry breaking of metal cluster-based strongly correlated systems can give rise to collective ***,the twodimensional Nb_(3) cluster compound Nb_(3)Cl_(8) is shown to suffer dramatic symmetry breaking and electron disproportionation under compression.A structural phase transition from trigonal P–3m1 to monoclinic C2/m is observed near 8 GPa with the three-fold symmetry *** disproportionation occurs on Nb_(3) clusters from delocalized Nb^(8/3+)Nb^(8/3+)Nb^(8/3+)to localized Nb^(3+)Nb^(3+)Nb^(2+),which results in a subtle bandgap discontinuity,as evidenced by electrical transport and UV-Vis absorption measurements.

关键词： Nb_(3)Cl_(8) symmetry breaking electron disproportionation layered semiconductor high pressure

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Pressure-Induced Topochemical Polymerization toward Advanced Energetic Materials

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CCS Chemistry 2023年第8期5卷 1815-1826页

作者： Guangyu Qi Siwei Song Zhiying Deng Dajian Huang Fang Chen Bingmin Yan Huiyang Gou Qinghua Zhang Yi Wang Institute of Chemical Materials China Academy of Engineering Physics(CAEP)Mianyang 621999 Center for High Pressure Science and Technology Advanced Research(hpstar) Beijing 100094

Pressure produces closely packed,high-density materials,thereby providing a promising strategy to obtain high-energy-density ***,new phases or structures of energetic materials at high pressure are often not quenchable under ambient *** this work,high-pressure topochemical methodology is first introduced for the preparation of stable energetic materials under ambient conditions.A pressure-induced polymerizable energetic material named PIP-1 is designed and *** experimental measurements demonstrate that the polymerization of PIP-1 is caused by the breakage of C≡C bonds and the generation of C=C *** accord with the experimental results,density functional theory calculations further revealed that the monomer PIP-1 is polymerized to generate 1D PIP-1 tape,and the density of polymerized PIP-1 is increased by 4.9%upon *** successful realization of high-energy-density structure using high pressure showcases a new design strategy for advanced polymerizable energetic materials.

关键词： high pressure energetic material topochemistry pressure-induced polymerization

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Intrinsic Zero-Linear and Zero-Area Compressibilities over an Ultrawide Pressure Range within a Gear-Spring Structure

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CCS Chemistry 2022年第10期4卷 3246-3253页

作者： Dequan Jiang Ting Wen Huimin Song Zimin Jiang Chen Li Ke Liu Wenge Yang Ho-kwang Mao Yonggang Wang Center for High Pressure Science and Technology Advanced Research(hpstar) Beijing 100094 School of Materials Science and Engineering Peking UniversityBeijing 100871

Materials with zero-linear compressibility(ZLC)and zero-area compressibility(ZAC)have great promise for specific applications retaining constancy in specific directions or planes under external *** date,no more than 10 ZLC/ZAC materials have been reported,most of which have very limited working pressure ranges(<10 GPa).Herein,we report the observation of ZLC and ZAC in Li2Ti(IO3)6 with a gear-spring type structure over an ultrawide pressure range(0–40 GPa).

关键词： high pressure zero-linear/zero-area compressibilities gear-spring mechanism ultrawide pressure range

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Phase Stability and Hydroxyl Vibration of Brucite Mg(OH)_(2) at High Pressure and High Temperature

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Chinese Physics Letters 2021年第3期38卷 111-115页

作者：桂维彬赵超帅刘锦 Center for High Pressure Science and Technology Advanced Research(hpstar) Beijing 100094China

Brucite Mg(OH)_(2) is an archetypal hydrous mineral and it has attracted a great deal of ***,little is known about the evolution of hydroxyl groups in brucite with respect to subduction *** carried out Raman measurements up to 15.4 GPa and 874 K via an externally heated diamond anvil cell,investigating the stability of brucite under the conditions relevant to subducting *** hydroxyl vibration mode A_(1g)(I) of brucite is weakened under simultaneous high pressure-temperature ***,the presence of carbonated solution can destabilize the hydroxyl groups of brucite at low *** results suggest that brucite releases water when reacting with hydrogen carbonate ion to form magnesite MgCO_(3) in subduction *** implies that the global water cycle is largely coupled with the deep carbon cycle in Earth’s interior.

关键词： hydroxyl cycle implies

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Deep mantle hydrogen in the pyrite-type FeO_(2)–FeO_(2)H system

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Geoscience Frontiers 2021年第2期12卷 975-981页

作者： Qingyang Hu Jin Liu Center for High Pressure Science and Technology Advanced Research(hpstar) Beijing100094China

The pyrite-type FeO_(2)and FeO_(2)H were synthesized at the pressure-temperature conditions relevant to Earth’s deep lower *** the water-iron reaction,the pyrite-phase is a good candidate to explain the chemical heterogeneities and seismological anomalies at the bottom of the *** solid solution of pyrite-type FeO_(2)and FeO_(2)H,namely the FeO_(2)Hx(0≤x≤1),is particularly interesting and introduces puzzling chemical states for both the O and H atoms in the deep *** the role of H in the FeO_(2)–FeO_(2)H system has been primarily investigated,discrepancies *** this work,we summarize recent progress on the pyrite-phase,including FeO_(2),FeO_(2)H,and FeO_(2)Hx,which is critical for understanding the water cycling,redox equilibria,and compositional heterogenicities in the deep lower mantle.

关键词： Deep lower mantle Core-mantle boundary Pyrite-type phase Hydrogen-bearing phase

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