Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Su Han,Li Jingru,Zhong Yu,Liu Yu,Gao Xuhong,Kuang Juner,Wang Minkang,Lin Chunxi,Wang Xiuli,Tu Jiangping
Sulfides are promising electrolyte materials for all-solid-state Li metal batteries due to their high ionic conductivity and machinability. However, compatibility issues at the negative electrode/sulfide electrolyte interface hinder their practical implementation. Despite previous studies have proposed considerable strategies to improve the negative electrode/sulfide electrolyte interfacial stability, industrial-scale engineering solutions remain elusive. Here, we introduce a scalable Li-Al-Cl stratified structure, formed through the strain-activated separating behavior of thermodynamically unfavorable Li/Li 9 Al 4 and Li/LiCl interfaces, to stabilize the negative electrode/sulfide electrolyte interface. In the Li-Al-Cl stratified structure, Li 9 Al 4 and LiCl are enriched at the surface to serve as a robust solid electrolyte interphase and are diluted in bulk by Li metal to construct a skeleton. Enabled by its unique structural characteristic, the Li-Al-Cl stratified structure significantly enhances the stability of negative electrode/sulfide electrolyte interface. This work reports a strain-activated phase separation phenomenon and proposes a practical pathway for negative electrode/sulfide electrolyte interface engineering.
研究领域:
材料科学
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电化学
·
电池技术
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Ming Lei,Yao Tang,Huimin Wang,Lihua Zhu,Guihua Zhang,Yu Zhou,Heqing Tang
It is still very difficult to achieve rapid cleavage of C-Cl bond of highly-chlorinated benzenes by catalytic reduction process under mild conditions. By using pentachlorobenzene (PentaCB) as a representative of highly-chlorinated benzenes, we proposed a strategy to achieve rapid and complete dechlorination of highly-chlorinated benzenes by exploiting palladium with low content deposited g-C 3 N 4 (Pd/g-C 3 N 4 ) as a catalyst with NaBH 4 as a reductant. Under favorable conditions, this strategy yielded a dechlorination efficiency of 100% for PentaCB (0.4 mmol L −1 ) in methanol solution at 30 °C within 20 min, and especially the consumption of NaBH 4 is as low as 10 mmol L −1 with a molar ratio of Cl atoms to NaBH 4 of only 1:5. A hydro-dechlorination pathway was confirmed to dominate the dechlorination of PentaCB, which involves active hydrogen species (H*) as being identified by electron spin resonance (ESR) monitoring and isotope labelling experiments. The dechlorination rate constant value of chlorobenzenes (CBs) was only a little dependent on the number of chlorine atoms and the chlorine atom with smaller steric hindrance was prior to be substituted by H*. A catalytic mechanism that Pd nanoparticles played an important role on both the weakening/breaking of C-Cl bond and the formation of active hydrogen species was further clarified: Pd exerts affinity interaction on chlorine atoms at ortho -position of CBs molecules to form adsorbed state [CBs] ads ; H* was formed on the Pd surface due to its strong ability in H* retainment; subsequently the generated H* attacks the C-Cl bond in [CBs] ads to achieve hydrodechlorination. The new method provides a highly efficient method to remove halogenated pollutants.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2017
·
IF 6.395
Bo Li,Yanan Zhang,Luyuan Zhang,Longwei Yin
Inorganic CsPbBr 3 perovskite is arousing great interest following after organic-inorganic hybrid halide perovskites, and is found as a good candidate for photovoltaic devices for its prominent photoelectric property and stability. Herein, we for the first time report on PbCl 2 -tuned inorganic Cl-doped CsPbBr 3 (Cl) perovskite solar cells with adjustable crystal structure and Cl doping for enhanced carrier lifetime, extraction rate and photovoltaic performance . The effect of PbCl 2 on the morphologies, structures, optical, and photovoltaic performance of CsPbBr 3 perovskite solar cells is investigated systemically. Compared with orthorhombic CsPbBr 3 , cubic CsPbBr 3 demonstrates a significant improvement for electron lifetime (from 6.7 ns to 12.3 ns) and diffusion length (from 69 nm to 197 nm), as well as the enhanced electron extraction rate from CsPbBr 3 to TiO 2 . More importantly, Cl doping benefits the further enhancement of carrier lifetime (14.3 ns) and diffusion length (208 nm). The Cl doped cubic CsPbBr 3 (Cl) perovskite solar cell exhibits a J sc of 8.47 mA cm −2 and a PCE of 6.21%, superior to that of pure orthorhombic CsPbBr 3 (6.22 mA cm −2 and 3.78%). The improvement of photovoltaic performance can be attributed to enhanced carrier lifetime, diffusion length and extraction rates, as well as suppressed nonradiative recombination.
研究领域:
材料科学
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光伏技术
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半导体物理
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产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 14
·5355
·
IF 4.6
Keyan Chen,Shiqi Fu,Chenyu Jin,Fan Guo,Yu He,Qi Ren,Xuesheng Wang
Smartphone-assisted fluorescence and colorimetric methods for the on-site detection of Hg2+and Cl−were established based on the oxidase-like activity of the Au–Hg alloy on the surface of Au/Cu/Ti3C2NSs. The Au nanoparticles (NPs) were constructed via in-situ growth on the surface of Cu/Ti3C2NSs and characterized by different characterization techniques. After the addition of Hg2+, the formation of Hg–Au alloys could promote the oxidization of o-phenylenediamine (OPD) to generate a new fluorescence emission peak of 2,3-diaminopenazine (ADP) at 570 nm. Therefore, a turn-on fluorescence method for the detection of Hg2+was established. As the addition of Cl−can influence the fluorescence of ADP, the fluorescence intensity was constantly quenched to achieve the continuous quantitative detection of Cl−. Therefore, a turn-off fluorescence method for the detection of Cl−was established. This method had good linear ranges for the detection of Hg2+and Cl−in 8.0–200.0 nM and 5.0–350.0 µM, with a detection limit of 0.8 nM and 27 nM, respectively. Depending on the color change with the detection of Hg2+and Cl−, a convenient on-site colorimetric method for an analysis of Hg2+and Cl−was achieved by using digital images combined with smartphones (color recognizers). The digital picture sensor could analyze RGB values in concentrations of Hg2+or Cl−via a smartphone app. In summary, the proposed Au/Cu/Ti3C2NSs-based method provided a novel and more comprehensive application for environmental monitoring.Keywords:Au/Cu/Ti3C2NS;Au–Hg alloy;oxidase-like activity;smartphone;colorimetric detection
研究领域:
环境科学
·
分析化学
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材料科学
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纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
LANGMUIR
·
2023
·
IF 3.9
Hongqi Nie,Zikangping Wang,Xue-Xue Zhang,Su-Lan Yang,Zhi Ren,Qi-Long Yan
In this study, a 2D structured triaminoguanidine-glyoxal polymer with a high nitrogen content has been coordinated with metal ions to produce energetic metal complexes (TAGP-Ms) employed as energetic burn rate inhibitors. The metal ions (Ba2+, K+, and Ca2+) are elaborately selected based on their ability of suppressing the burn rate of composite propellants. The CL-20 crystals were intercalated with prepared TAGP-Ms materials via a solvent–antisolvent method for realization of the precise control on burning behaviors of studied propellants. The influence of TAGP-Ms inhibitors on thermal decomposition and combustion characteristics of high-energy composite propellants was evaluated using thermal analysis and a combustion diagnostic method. Results of TGA/DSC-FTIR measurements suggest that the thermal decomposition of CL-20-containing composite propellants was found to be constrained by varied degrees as a result of TAGP-Ms additions, in which the TAGP-K displays a stronger effect on suppressing the thermal decomposition of CL-20 compared with that of other TAGP-Ms. The FTIR spectra indicate that the primary gaseous phase products are composed of N2O, H2O, and CO2 in CL-20 decomposition, as well as by HCl, H2O, NO2, and N2O in the decomposition of AP for all studied composite propellants. The combustion characterizations show that the TAGP-K-containing composite propellant exhibits a significantly reduced rate of heat release but is associated with a higher flame radiation intensity increased by 4.2% compared with that of the reference propellant, which clearly implies that the TAGP-K is capable of suppressing the energy release rate while ensuring the high energetic features of propellants to be well maintained. Moreover, the burn rate pressure exponents are considerably decreased by ∼10% for the TAGP-K-containing propellants in comparison with those of propellants with the typical formulation, which strongly suggests that TGAP-Ms are promising candidates for tuning the combustion behaviors of composite propellants by influencing the decomposition processes of CL-20 and AP collectively.
研究领域:
材料科学
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燃烧与爆炸学
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产品关联
DOI
PubMed
高影响因子
Scientific Reports
·
2022
·Vol. 12
·期 1
·1-10
·
IF 4.996
Tan Meina,Qin Yang,Wang Yiping,Zhang Fazhi,Lei Xiaodong
We propose a new Cu–Al dual-ion battery that aqueous solution composed of LiCl, CuCl and AlCl 3 (LiCuAl) is used as the electrolyte, CuS is used as the cathode of aqueous aluminum ion battery for the first time and copper foil is used as the anode. The assembled Cu–Al dual-ion battery yields a reversible capacity of 538 mA h/g at 200 mA/g, and exhibits longterm cycling stability of over 200 cycles with 88.6% capacity retention at 1000 mA/g. Above excellent performance is inseparable from the three components of LiCuAl electrolyte and electrode materials. The Al-storage mechanism of CuS is proposed that the S–S bond in CuS lattice interacts with aluminum ions during the aluminum storage process. In addition, the charging and discharging process does not cause irreversible damage to the S–S bond, thus Cu–Al dual-ion battery with CuS as cathode shows great cycle stability.
研究领域:
电化学
·
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2019
·
IF 7.149
Yu Lei,Shuangshuang Cheng,Na Luo,Xin Yang,Taicheng An
Cl• and Cl2•– radicals contribute to the degradation of trace organic contaminants (TrOCs) such as pharmaceutical and personal care products and endocrine-disrupting chemicals. However, little is known about their reaction rate constants and mechanisms. In this study, the reaction rate constants of Cl• and Cl2•– with 88 target compounds were determined using laser flash photolysis. Decay kinetics, product buildup kinetics, and competition kinetics were applied to track the changes in their transient spectra. Cl• exhibited quite high reactivity toward TrOCs with reaction rate constants ranging from 3.10 × 109 to 4.08 × 1010 M–1 s–1. Cl2•– was less reactive but more selective, with reaction rate constants varying from <1 × 106 to 2.78 × 109 M–1 s–1. Three QSAR models were developed, which were capable of predicting the reaction rate constants of Cl2•– with TrOCs bearing phenol, alkoxy benzene, and aniline groups. The detection of Cl•-adducts of many TrOCs suggested that Cl• addition was an important reaction mechanism. Single electron transfer (SET) predominated in reactions of Cl• with TrOCs bearing electron-rich moieties (e.g., sulfonamides), and their cation radicals were observed. Cl• might also abstract hydrogen atoms from phenolic compounds to generate phenoxyl radicals. Moreover, Cl• could react with TrOCs through multiple pathways since more than one transient intermediate was detected simultaneously. SET was the major reaction mechanism of Cl2•– reactions with TrOCs bearing phenols, alkoxy benzenes, and anilines groups. Cl2•– was found to play an important role in TrOC degradation, though it has been often neglected in previous studies. The results improve the understanding of halogen radical-involved chemistry in TrOC degradation.
研究领域:
环境化学
·
化学动力学
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物理化学
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水处理技术
·
有机化学
✓ 已验证
DOI
高影响因子
COMBUSTION AND FLAME
·
2025
·
IF 6.2
Yanggang Huang,Yong Kou,Ting Chang,Jiaqi Wei,Hongfei Liu,Lei Xiao,Wei Jiang,Gazi Hao
Aiming at the critical issues of uneven dispersion, inadequate interfacial contact, and significant mass/heat transfer resistance inherent in the mechanical mixing process for traditional solid propellant charging, this study proposes a novel strategy for constructing energetic micro-units through core-shell structural design, with the aim of achieving highly reactive and integrated composites tailored for practical solid propellant applications. Using etched aluminum (Al) powder as the core and ammonium perchlorate (AP) together with hexanitrohexaazaisowurtzitane (CL-20) as the composite shell, Al@AP/CL-20 micro-units with uniform coatings of AP/CL-20 and well-defined core-shell structures were successfully fabricated via solvent evaporation. The thermogravimetric-differential scanning calorimetry (TG-DSC) and combustion analyses indicate that Al@AP/CL-20 energetic micro-units exhibit significantly earlier decomposition peak temperature compared to pure AP, larger and more concentrated exothermic peaks, as well as stronger combustion intensity and higher flame temperature than the Al/AP/CL-20 composite in the physical mixture. The result confirms that the Al@AP/CL-20 composite structure can effectively enhance the synergistic effect between components, thereby improving the performance of the micro-units. Moreover, as the etching time increases, the porosity of the Al powder surface rises, leading to a further enhancement in the combustion performance of the Al@AP/CL-20 energetic micro-unit. In particular, when the Al powder etching time reached 5 h and the mass ratio of Al/AP/CL-20 was 1:2:2, the Al@AP/CL-20 micro-units demonstrated the best combustion performance, with the highest light intensity and a maximum flame temperature of 1094 °C — a 49 % improvement over the physically blended sample (PAAC-2) with the same mass ratio. This is attributed to the well-defined core-shell structure, which significantly shortens mass and heat transfer distances between components, and a better-matched oxygen balance that imparts the best combustion efficiency. The study affirms that the core-shell energetic micro-unit strategy effectively overcomes the limitations of conventional mixing methods and provides a pathway for formulating highly reactive solid propellant with enhanced energy release efficiency.
研究领域:
材料科学
·
推进剂化学
·
纳米复合材料
·
燃烧学
·
热力学
·
功能材料
·
能源材料
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL PHYSICS LETTERS
·
2023
·
IF 2.8
Wei Li,Xianhua Sheng,Zhaoliang Yu,Qian Tang,Jinghua Geng,Dangzheng Hu,Xiangdong Meng,Yumei Zhang
Co-based compound is a kind of bifunctional electrocatalyst for the half reactions of water splitting. Here we report the catalytic performance of Co-Cl-C composited catalyst prepared by flash Joule heating system in oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). It is found that Co-Cl-C composited film is an efficient electrocatalyst of OER and HER. In addition, the flash Joule heating is a fast, low energy consumption, and environmentally friendly preparation method. It opens up a new idea for the preparation method of composite materials.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Jin Chen,Xuelong Lv,Wenjian Xu,Xiaolan Li,Jing Chen,Hongpeng Jia
The exploit of simple method to synthesize and recover catalyst is meaningful to widespread application of environmental catalysis. Different from traditional knowledge about deposition of Ag cation by Cl anion, we find that Cl anion coordinates with Ru and Ag cations simultaneously to micro-micelles and results in homogeneously alloying of bimetals. The Ru-Ag alloy exhibits a remarkable activity and stability in propane catalytic oxidation at moderate condition, but is still inactivated by extremely-high temperature and humidity due to metal sintering and oxidation as well as support reconstruction. Fortunately, utilization of Cl coordination to extract and combine bimetals at redox condition is proved as a feasible and simple way to regenerate the thermally-inactivated catalyst. With in-situ characterization, the synergic effect between Ru and Ag on propane oxidation obeying Mars-van-Krevelen mechanism is revealed. Through monolith test, the practice application of Ru-Ag catalyst prepared via Cl-assisted method is thought to be promising.
研究领域:
催化
·
环境化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Peng Bao,Su Jiang,Yang Chen,Yuanlin Fan,Yaning Li,Boliang Wang
Despite the extensive researches on CL-20 crystals, the mechanical safety issues and process problems of CL-20 applications have not been studied in-depth. Herein, the cellulose nanocrystals (CNC) was doped in microcrystalline wax (MW), oxidized microcrystalline wax (OMW) and hydrogel (PPC) to design and fabricate the cross-linked CL-20 composites by simple water-suspension melting and freeze-drying methods. The composites were characterized by SEM, XPS, TG-DSC, XRD, mechanical sensitivity device and inclined chute tester. It is found that the CNC@OMW composite film exhibits excellent coating effect (99.96%) on CL-20 due to the cross-linking results. The E a of CL-20 is increased from 190.92 to 388.71 kJ/mol under the synergistic effect of the excellent compatibility between components and the compact coating structure of CNC@OMW. Additionally, the film enhances the T p0 of CL-20 from 218.15 to 222.66 ℃ and T b from 220.27 to 223.73 ℃, respectively. While, the PPC@CNC only promoted E a , T p0 and T b of CL-20–292.89.71 kJ/mol, 224.22 ℃ and 225.66 ℃, respectively. Besides, the XRD results confirms that three composite films dose not cause a transformation of the ε- CL-20 crystal phase. Most importantly, the cross-linked film brings mechanical sensitivity of CL-20 from 60 N and 3.5 J to a level of over 360 N and 10.4 J, comparable to WO 3 /Al nanothermite with 5 wt% polyaniline (360 N) and composite with 95 wt% LLM-105 and 5 wt% ternary (11–12 J). This improvement enables the composite explosives to be handled using standard procedures. Furthermore, the ability of the particles to accumulate electrostatic charge after cross-linking coating is significantly reduced, and PVC is more suitable as the contact material of CL-20 and composite particles than copper for use in the transportation and packaging. These findings can serve as a reference for wide application of CL-20.
研究领域:
材料科学
·
炸药工程
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Daqin Chen,Junni Li,Xiao Chen,Jiangkun Chen,Jiasong Zhong
Currently, metal halide perovskite nanocrystals have been extensively explored due to their unique optoelectronic properties and wide application prospects. In the present work, a facile grinding method is developed to prepare whole-family APbX3 (A = MA, FA, and Cs; X = Cl, Br, and I) perovskite nanocrystals. This strategy alleviates the harsh synthesis conditions of precursor dissolution, atmosphere protection, and high temperature. Impressively, the as-prepared perovskite nanocrystals are evidenced to have halogen-rich surfaces and yield visible full-spectral emissions with maximal photoluminescence quantum yield up to 92% and excellent stability. Additionally, the grinding method can be extended to synthesize widely concerned Mn2+-doped CsPbCl3 nanocrystals with dual-modal emissions of both excitons and dopants. As a proof-of-concept experiment, the present perovskite nanocrystals are demonstrated to be applicable as blue/green/red color converters in UV-excitable white-light-emitting diodes.
研究领域:
材料科学
·
纳米技术
·
光电
✓ 已验证
产品关联
DOI
PubMed
高影响因子