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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Thermoelectric Transport Performance in p-Type AgSbTe2-Based Materials through Entropy Engineering

Abdul Basit,Tanveer Hussain,Xin Li,Jiwu Xin,Bin Zhang,Xiaoyuan Zhou,Guoyu Wang,Ji-Yan Dai

Being a major obstacle, Ag2Te has always been restricted in p-type AgSbTe2-based materials to improve their thermoelectric performance. This work reveals a stabilized AgSbTe2 through Sn/Ge alloying as synthesized by melting, annealing, and hot press. Interestingly, addition of Sn/Ge in AgSbTe2 extended the solubility limit up to ∼30% and hence suppressed Ag2Te in Ag(1–x)SnxSb(1–y)GeyTe2 compounds and led to enhanced electrical transport. Moreover, electrical and thermal transport properties of AgSbTe2 have been greatly affected by the phase transition of Ag2Te near 425 K. However, high-entropy Ag0.85Sn0.15Sb0.85Ge0.15Te2 compound results in a stabilized rock-salt structure and presents a high power factor of ∼10.8 μW cm–1 K–2 at 757 K. Besides, density functional theory reveals that available multivalence bands in Sn/Ge-doped AgSbTe2 lead to reduction in energy offsets. Meanwhile, a variety of defects appear in the Ag0.85Sn0.15Sb0.85Ge0.15Te2 sample due to entropy change, and thus lattice thermal conductivity decreases. Ultimately, a high figure of merit of ∼1.5 is attained at 757 K. This work demonstrates a roadmap for other group IV–VI materials so that the high-entropy approach may inhibit the impurity phases with extended solubility limit and result in high thermoelectric performance.

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ACS Nano · 2024 · IF 15.8

Three-Dimensional Metal–Organic Framework@Cellulose Skeleton-Reinforced Composite Polymer Electrolyte for All-Solid-State Lithium Metal Battery

Xin Song,Kang Ma,Jian Wang,Han Wang,Haijiao Xie,Zongmin Zheng,Jianmin Zhang

High-safety and high-energy-density solid-state lithium metal batteries (SSLMBs) attract tremendous interest in both academia and industry. Especially, composite polymer electrolytes (CPEs) can overcome the limitations of single-component solid-state electrolytes. In this work, a strategy of combining a rigid functional skeleton with a soft polymer electrolyte to prepare reinforced CPEs was adopted. The in situ grown zeolitic imidazolate frameworks (ZIFs) with three-dimensional cellulose fiber skeleton (ZIF-67@CF) and succinonitrile (SN) plasticizer into poly(ethylene oxide) (PEO) together form ZIF-67@CF/PEO-SN CPEs. The addition of ZIF-67@CF and SN to PEO synergistically enhanced the physical and electrochemical properties of CPEs. Furthermore, the conduction mechanism of lithium-ion (Li+) in CPEs was studied using density functional theory. It is impressive that the ZIF-67@CF/PEO-SN CPEs at 30 °C exhibit a high ionic conductivity of 1.17 × 10–4 S cm–1, a competitive Li+ transference number of 0.40, a wide electrochemical window of 5.0 V, a notable tensile strength of 18.7 MPa, and superior lithium plating/stripping stability (>550 h at 0.1 mA cm2). Such favorable features endowed LiFePO4/(ZIF-67@CF/PEO-SN)/Li cell at 30 °C with a high discharging capacity (152.5 mA h g–1 at 0.2 C), a long cycling lifespan (>150 cycles with 99% capacity retention), and superior operating safety. This work provides insights and promotes the application of functionalized CPEs for SSLMBs.

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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2024 · IF 11.2

Ti3C2Tx MXene enhanced PEO/SN-based solid electrolyte for high-performance Li metal battery

Hao Xu,Shuai Liu,Zhiang Li,Fan Ding,Ting Wang,Ting Liu,Weimin Wang,Kaikai Song,Jie Liu,Lina Hu

Succinonitrile has shown significant promise for application in polymer electrolytes for solid-state lithium metal batteries due to its high ionic conductivity at low-temperature. However, the use of Succinonitrile is limited due to its corrosion of Li metal. Herein, we report a solid polymer electrolyte with high ionic conductivity (2.17 × 10 −3 S cm −1 , 35 °C) enhanced by Ti 3 C 2 T x . Corrosion of the Li anode is prevented due to the Succinonitrile molecules being efficiently anchored by Ti 3 C 2 T x . Meanwhile, the coordination environment of Li + is weakened due to the introduction of competitive coordination induction effects into the polymer electrolyte, resulting in efficient Li + conduction. Furthermore, the mechanical properties of the electrolyte are enhanced by modulating the ratio of Ti 3 C 2 T x to suppress the growth of Li dendrites. Therefore, Li||Li symmetric batteries deliver stable cycling up to 8000 h at 28 °C. LiFePO 4 ||Li full batteries exhibit excellent cycling stability of 151.7 mAh g −1 with a capacity retention of 99.3% after 300 cycles. This work not only presents a new idea to suppress the corrosion of the Li anode by Succinonitrile but also provides a simple, feasible, and scalable strategy for high-performance Li metal batteries.

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Nanomaterials · 2024 ·Vol. 14 ·期 5 ·437 · IF 4.4

Polymer Lewis Base for Improving the Charge Transfer in Tin–Lead Mixed Perovskite Solar Cells

Yanjun Xing,Zhiqiang Deng,Qiuxiang Wang,Jiaxing Xiong,Xiaohui Liu,Like Huang,Yuejin Zhu,Jing Zhang

The poor film stability of Sn-Pb mixed perovskite film and the mismatched interface energy levels pose significant challenges in enhancing the efficiency of tin–lead (Sn-Pb) mixed perovskite solar cells. In this study, polyvinylpyrrolidone (PVP) is introduced into the PVK perovskite precursor solution, effectively enhancing the overall stability of the film. This improvement is achieved through the formation of robust coordination bonds between the carbonyl (C=O) in the pyrrole ring and the undercoordinated SnIIand PbII, thereby facilitating the passivation of defects. Furthermore, the introduction of PVP inhibits the oxidation of tin (Sn), thereby enhancing the n-type characteristics of the perovskite film. This adjustment in the energy level of the PVK perovskite film proves instrumental in reducing interface energy loss, subsequently improving interface charge transfer and mitigating device recombination. Consequently, perovskite solar cells incorporating PVP achieve an outstanding champion power conversion efficiency (PCE) of 21.31%.

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Materials · 2024 ·Vol. 17 ·期 19 ·4809 · IF 3.1

Preparation and Electrothermal Transport Behavior of Sn8[(Ga2Te3)34(SnTe)66]92 Bulk Glass

Yaqi Zhang,Feng Guo,Huan Zhang,Mingming Zhang,Jianxiu Su,Zhengxin Li

High-conductivity tellurium-based glasses were anticipated to be the attractive candidates in chalcogenide glass systems on account of their distinctive characteristics and extensive application prospects. In this paper, the high-density (>96%) Sn8[(Ga2Te3)34(SnTe)66]92bulk glass with the density of 5.5917 g/cm3was successfully prepared by spark plasma sintering (SPS) technology at 460 K, using a 5 min dwell time and 450 MPa pressure. The room-temperature thermal conductivity of Sn8 bulk materials significantly decreased from 1.476 W m−1∙K−1in the crystalline sample to 0.179 W m−1∙K−1in the glass, and the Seebeck coefficient obviously increased from 35 μV∙K−1in to 286 μV∙K−1, indicating that the glass transition of tellurium-based semiconductors could optimize the thermal conductivity and Seebeck coefficient of the materials. Compared to the conventional tellurium-based glassy systems, the fabricated Sn8 bulk glass presented a high room-temperature conductivity (σ =6.2 S∙m−1) and a large glass transition temperature (Tg=488 K), which was expected to be a promising thermoelectric material.

CAS / MDL: 7440-31-5 12040-02-7
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CRYSTENGCOMM · 2024 ·Vol. 26 ·期 10 ·1418-1429 · IF 2.6

Preparation and growth mechanism of centimeter-scale (AgxCu1−x)2ZnSnS4 single crystals via a molten salt method

Jun Liao,Sihao Ye,Xupeng Zhu,Wenfeng Fu,Shuwen Xue,Jing Qi,Jun Zhang

Kesterite Cu2ZnSnS4 (CZTS) is considered as one of the most promising thin-film solar cell and photocatalytic materials; however, its efficiency in practical photoelectric applications is often seriously limited by the presence of large numbers of Cu–Zn antisite defects. Alloying with Ag to fabricate Ag-alloyed CZTS ((AgxCu1−x)2ZnSnS4, ACZTS) can reduce the Cu–Zn antisite defects in CZTS, but few research studies have been able to separately clarify the effect of Ag content and growth temperature on large-sized (AgxCu1−x)2ZnSnS4 single crystals. In this study, centimeter-scale high-quality ACZTS single crystals were synthesized via an Ag-alloying strategy by a molten salt method for the first time. The results showed that the synthesized ACZTS have a high-quality single-crystal structure. A series of experiments was performed using various characterization techniques and it was found that Ag content and growth temperature were crucial in determining the size of ACZTS single crystals obtained through a molten salt method and that the associated CZTS base generated at high temperature was beneficial for further ACZTS single-crystal growth in this high-temperature environment. The experimental results showed that the growth mechanism of ACZTS crystals prepared using a molten salt method could be attributed to a type of epitaxial growth process. Our study provides a promising approach for growing large-sized ACZTS single crystals with high quality that can provide a potential single-crystal platform for the study of light-emitting diodes, photocatalytic hydrogen production, etc.

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APPLIED CATALYSIS B-ENVIRONMENTAL · 2024 · IF 20.2

Revealing the nontrivial topological surface states of catalysts for effective photochemical carbon dioxide conversion

Kangwang Wang,Longfu Li,Peifeng Yu,Nannan Tang,Lingyong Zeng,Kuan Li,Chao Zhang,Rui Chen,Zaichen Xiang,Huichao Wang,Yongqing Cai,Kai Yan,Huixia Luo

Topological semimetals with protected surface states mark a new paradigm of research beyond the early landmarks of band-structure engineering, allowing fabrication of efficient catalyst to harness the rich metallic surface states to activate specific chemical processes. Herein, we demonstrate a facile solid-phase method for in-situ doping of Ir at the Os sites in the Os 3 Sn 7 , an alloy with topological states, which significantly improves the photocatalytic performance for the reduction of CO 2 to CO and CH 4 . Experimental evidence combined with theoretical calculations reveal that the nontrivial topological surface states greatly accelerate charge-separation/electron-enrichment and adsorption/activation of CO 2 molecules, rendering highly efficient reaction channels to stimulate the formation of *COOH and *CO, as well CHO*. This work shows the promise of achieving high photocatalytic performances with synthesizing topological catalysts and provides hints on the design of novel topological catalysts with superior photoactivity towards the CO 2 reduction reaction.

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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2025 · IF 5.4

Self-assembly of phosphorus-containing ionic liquids on black phosphorus nanosheets for enhancing the fire safety of ethylene-vinyl acetate copolymers

Hao Huang,Yueyue Yu,Qian Geng,Tianhao Zhang,Mingqiang Yan,Dong Feng,Delong Xie

This study presents the design and synthesis of a novel phosphorus-containing ionic liquid flame retardant, DV, which serves as both a surfactant and a synergistic flame retardant. DV self-assembled onto the surface of BP nanosheets through electrostatic interactions, forming a polymerized ionic liquid coating via radical initiation. Simultaneously, DOPO-derived groups were incorporated into the polymer matrix by ionic bonding with imidazole groups, further enhancing the structural integrity of the composites. The resulting composite was used to develop EVA-based materials with outstanding mechanical properties and flame retardancy. At a low loading of 3 wt% DVBP, the synergistic effect of phosphorus and nitrogen, combined with the two-dimensional structure of BP, facilitated char formation at elevated temperatures, effectively inhibiting the transfer of oxygen and flammable substances. Additionally, the gas-phase flame-retardant mechanism reduced the release of pyrolysis products. The composite achieved a V-0 rating in the UL-94 test, a 22.3 % reduction in peak heat release rate (PHRR), and an 8.1 % increase in tensile strength, highlighting its potential for application in cables used in critical transport equipment.

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Inorganic Chemistry Frontiers · 2024 · IF 6.1

Tailoring supertetrahedral cadmium/tin selenide clusters into a robust framework for efficient elimination of Cs+, Co2+, and Ni2+ ions

Kai-Yao Wang,Meng-Yu Li,Lin Cheng,Xin Hao,Cheng Wang

Long-lived 137Cs/134Cs, 60Co, and 63Ni with high-energy β/γ emissions are primary toxic fission/activation products in nuclear-contaminated water, causing irreversible damage to the ecological environment and human health. Rapid remediation of these radionuclides emerges as an urgent task, while the deficiencies in adsorption kinetics, selectivity and acid resistance hinder the material innovation for practical applications. Herein, we have developed a hybrid cadmium/tin selenide adsorbent K3.4(CH3NH3)0.45(NH4)0.15Cd2Sn3Se10·3.4H2O (CdSnSe-2K) for the enrichment and sequestration of Cs+, Co2+, and Ni2+ ions. CdSnSe-2K features a unique open-framework constructed from the interlinkage of T2-{M4Se10} (M = SnIV/CdII) supertetrahedral clusters and M bridges, accelerating the ion transfer in the tunnel system and thus affording quick kinetics (k2 = 9.706, 0.182, 0.099 g mg−1 min−1 for Cs+, Co2+, Ni2+). Remarkably, the removal rate RCs increases to 98.54% in just 2 min and 99.57% in 5 min (equilibrium), which is responsible for an ultra-high distribution coefficient Kd of 2.31 × 105 mL g−1. The soft-Lewis basic Se component endows CdSnSe-2K with a fantastic adsorption selectivity for Cs+, Co2+, and Ni2+ against various coexisting cations and anions in complex actual water environments even including the highly salty sea water medium. CdSnSe-2K exhibits a fantastic acid/base tolerance over pH = 2–13, and the maximum adsorption capacities qCsm, qCom and qNim under neutral condition are 218.08 ± 80.08, 43.95 ± 16.57 and 42.53 ± 16.50 mg g−1, respectively. In addition, CdSnSe-2K single crystals were also employed as the stationary phase for the fabrication of an ion exchange column, which shows an elimination efficiency above 99% in the long-term filtration for Cs+ (8200 BVs), Co2+ (4000 BVs) and Ni2+ (4000 BVs). This work not only highlights CdSnSe-2K as a promising Cs+, Co2+, and Ni2+ scavenger in radionuclide remediation, but also provides a supertetrahedral cluster-based construction strategy for open-framework selenide materials with enhanced adsorption kinetics, selectivity, and acid resistance.

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IEEE ELECTRON DEVICE LETTERS · 2024 · IF 4.1

SnS2-BN/SnSe Tri layer Heterojunctions for High Responsivity and Low Dark Current Self-Powered Near violet Detector

Xiyu Jia,Weishuai Duan,Mingchen Xu,Gaoning Fan,Pengyu Zhou,Yonghui Zhang,Hongxing Zheng,Mengjun Wang,Chao Fan

Near-violet (NV) detectors based on two-dimensional materials have attracted much attention due to their atomic-scale thickness and various band gaps. Among them, tin disulfide (SnS 2 ) has demonstrated significant potential for high-performance NV detectors due to its unique photoelectric properties. However, SnS 2 -based NV detector still have drawbacks such as low responsivity and high dark current. In this work a tri-layer van der Waals heterojunction of tin disulfide/h-boron nitride/tin selenide (SnS 2 /h-BN/SnSe) is proposed. The detector based on such tri-layer heterojunction exhibits an excellent self-powered detection performance to 405-nm NV illumination with a responsivity of 1.5 AW -1 , a low dark current of 2.6 pA, and a high fill factor of 51.8%, superior to detectors based on SnS 2 /SnSe bi-layer heterojunctions and most other two-dimensional materials. This study provides an efficient optimizing strategy for SnS 2 -based self-powered detector, thereby offering an opportunity for implementing innovation in NV detectors.

CAS / MDL: 7440-31-5
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY · 2024 ·Vol. 107 ·期 10 ·6911-6920 · IF 3.5

Synthesis of glucose-derived MAX phases and investigation on the phase evolution behavior

Ruixue Bai,Mian Li,Lingyan Feng,Qing Huang

The family of MAX phases and their two-dimensional derivative MXenes attract significant attention due to their unparalleled properties. Synthesis of MAX phases and MXene from biomass sources is important to expand their biology-related applications, while it remains a challenge. The present work explores the possibility to synthesize MAX phases and subsequently derive MXenes by using biomass precursor. Ti 3 AlC 2 MAX phase was synthesized by using glucose as the carbon source in molten salt. The conversion behavior from glucose to Ti 3 AlC 2 was investigated, and the conversion rate of carbon from glucose reached to 70.4% by optimizing the reaction conditions. The as-obtained Ti 3 AlC 2 can be derived into Ti 3 C 2 T x MXene and MXene quantum dots by common chemical treatments, which provides possibility for biomass-derived nanolaminates applying in biological applications such as biological catalysis, bioinstrumentation, and biological tracking.

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ACS Applied Energy Materials · 2025 · IF 5.5

Surficial Regulation of LLZO for High Performance Composite Solid Electrolyte

Zhen Zeng,Shengnan Zhang,Jun Cheng,Yuanyuan Li,Hongqiang Zhang,Xuan Zhou,Haonan Wang,Lijie Ci,Deping Li

Composite solid electrolytes (CSEs) based on inorganic oxide electrolyte and organic polymer electrolyte are recognized as promising candidates to realize high-performance solid state Li metal battery. Although the ionic conductivity of CSEs is limited, the usage of a plasticizer can make a great difference. Due to the high conductivity and extraordinary resistance to electrochemical oxidation, succinonitrile (SN) is widely used as a plasticizer in CSEs. However, the influence of the compatibility between SN and conductive oxide ceramics is underrated. In this work, we solve the catalytic decomposition effect of Li7La3Zr2O12 (LLZO) toward SN by silane coupling agent coating. Due to good affinity and chemical bonding toward the organic phase, the coating layer can promote the Li+ exchange rate through the heterogeneous interface between the organic/inorganic phase and improve the ionic conductivity of CSEs. Besides, surficial carbonyl groups of LLZO introduced by a coating can regulate the Li+ coordination structure and accelerate the ion transport. Our design realizes a high conductivity of 5.9 × 10–4 S cm–1 at 30 °C and enables the cyclability of Li symmetric cell over 480 h at 0.1 mA cm–2. Besides, the full cell with LiFePO4 (LFP) as the cathode delivers a capacity of 137.6 mAh g–1 with a capacity retention of 96.1% after 150 cycles. Our work demonstrates the regulation effect of interfacial structure on the electrochemical performance of SN-based CSEs, which contributes to realizing a practical solid state Li metal battery.

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