ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Yifan Zhou,Aosong Gao,Mingqiu Duan,Xiaoqi Zhang,Muzi Yang,Li Gong,Jian Chen,Shuqin Song,Fangyan Xie,Hao Jia,Yi Wang
Garnet-type Li6.4La3Zr1.4Ta0.6O12 (LLZTO) is a highly promising solid-state lithium metal battery electrolyte due to its exceptional ionic conductivity and electrochemical stability. However, when exposed to air, a passivation layer can be spontaneously formed on the garnet-type electrolyte, deteriorating its wettability with metallic lithium (Li) and impeding the lithium ion transfer at the Li–garnet electrolyte interface. The passivation layer is considered a critical issue for garnet-type solid electrolytes. Despite intensive research, the formation mechanism of the passivation film remains poorly understood. The key to elucidating the formation mechanism is to obtain a pristine garnet electrolyte surface and study how the pristine garnet electrolyte interacts with air. In this study, different passivation layer removal pretreatments were performed to expose pristine garnet electrolytes, and their impacts on the samples were systematically studied. The results reveal the overlooked negative impacts of vacuum annealing and acid treatment on LLZTO, which are indicated by the severe loss of Li and O and the formation of additional Li-depleted metal oxides. It was confirmed that argon annealing is the only viable approach to remove the passivation layer without introducing concomitant contaminations to LLZTO. Based on this method, we directly evidenced the formation of LiOH on LLZTO under rarefied air using quasi-in situ X-ray photoelectron spectroscopy. It was confirmed that the loss of Li and O ions, rather than Li+/H+ exchange, drives the formation of LiOH in the passivation layer. These results not only provide a better understanding of the surface and interface chemistry of LLZTO but also reveal a reliable surface treatment for the LLZTO sample.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Xin Liu,Xiaosong Zhang,Lan Li,Jianping Xu,Shuili Yu,Xiaokai Gong,Jiajia Zhang,Hao Yin
Perovskite quantum dots (PQDs) are among the most important luminescent semiconducting materials; however, they are unstable. Exposure to light, heat, and air can lead to irreversible degradation, which results in fluorescence quenching. Therefore, defects in PQDs significantly limit their practical application. Herein, we describe a simple method to enhance the photostability of CsPbBr3/nCdS QDs, which involves doping their shells with aluminum. The temperature-dependent photoluminescence (PL) of colloidal CsPbBr3/nCdS/Al2O3 QDs is investigated, and the thermal quenching of PL, blue shift of the optical band gap, and PL line width broadening are observed in each QD sample. Al2O3 layers on the CsPbBr3/nCdS QDs can effectively prevent photodegradation. Nonlinear, temperature-dependent exciton–phonon coupling and lattice dilation leads to radiative and nonradiative relaxation processes at temperatures ranging from 10 to 300 K; moreover, changes in the band gap and PL spectral line broadening are observed.
研究领域:
材料科学
·
光学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 21
·2112645
·
IF 19.924
Maogen Zhu,Zhechen Fan,Kangli Xu,Yuting Fang,Wei Sun,Yongchun Zhu
Lithium-metal batteries show great promise as the next generation rechargeable batteries with high theoretical energy density. Unfortunately, Li metal anodes suffer from serious corrosion of the electrolyte and by-products shuttled from cathode during cycling, such as O 2 in Li-O 2 batteries. Here, an oxygen-resistant and self-eliminating passivated layer is fabricated through a Wurtz-type reaction between Li metal and dichlorodimethylsilane (DCDMS). This passivated layer guarantees Li metal great stability with O 2 and inhibits the dendritic growth by eliminating the unpredictable fresh Li dendrites in their infancy stage. In addition, this passivated layer is constructed of LiCl and Poly(dimethylsilylene) phases, which provide good Li + transport, self-eliminate the undesirable by-products. The symmetric battery with this protective layer can achieve a stable Li plating/stripping with 500 h at O 2 atmosphere. Consequently, the Li-O 2 battery can maintain a stable cycling with more than 200 times and the Li||NCM811 battery presents excellent cycling performance (300 cycles at 0.5 C) and rate capacity (130.3 mA h g −1 at 5 C). This work provides both material and method breakthroughs for the development of electrode protection, which promotes the practical application of silanes and its ramification in alkali metal batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Guang-En Yuan,Yan-Ge Ma,Yunjie Qin,Yanbin Wang,Yunbei Li,Xin Zhang,Fenglin Yang
Zero-valent iron (ZVI) is widely used in the field of wastewater treatment and groundwater remediation, but it suffers from low reactivity due to the surface passivation layer. In the present work, bisulfite was used as an additive to enhance the reduction activity of ZVI under anoxic conditions. It was found that the reaction kinetic constant of p-nitrophenol reduction in ZVI/bisulfite process was approximately 132 times higher than that by ZVI alone. Bisulfite could dissolve and reduce some iron oxide on the ZVI surface, resulting in the exposure of more active sites like Fe 0 and Fe(II) for p-nitrophenol reduction through direct electron transfer. Common substances in water had no effects on p-nitrophenol degradation by ZVI/bisulfite process, but phosphate suppressed ZVI corrosion seriously. This work provides a simple, cost-effective and environmental-friendly method to improve the reducing activity of ZVI under anoxic conditions.
研究领域:
环境科学
·
废水处理
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Yuxiang Shi,Lei Li,Wei-xian Zhang,Shaolin Li
Zero-valent iron (ZVI) is a solid reductant that can react with a wide array of contaminants; however, its effectiveness is significantly reduced by the surface passivation layer formed on its surface. This study introduces mechanochemical depassivation to revitalize passivated ZVI and restore its reactivity. The method is exemplified through mechanical milling to depassivate ZVI with different passivation layers formed in solutions containing Cr(VI), Ni(II), and/or trichloroethylene, as well as in a complex water matrix. The results demonstrate rapid restoration of ZVI reactivity within 10 min of milling, achieving a 7-fold increase in contaminant removal capacity after eight cycles. The method universally outperforms acid pickling and ultrasonication across all of the tested passivation scenarios. Mechanistic analysis attributes its efficacy to the ductile–brittle disparity between the metallic iron and the passivation layers: brittle passivation layers fragment under mechanical stress, while ductile iron resists structural damage. Discrete element method simulations provide further mechanical insights into the milling dynamics and identify the contact frequency as the key factor determining depassivation efficiency. The study provides a versatile, environmentally benign, and effective depassivation method for ZVI reactions that can be integrated into ZVI reuse processes for water treatment applications.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Xin Wang,Yuzhu Pan,Yubing Xu,Tao Pang,Ziyu Wei,Dan Zhang,Ziyi Liu,Byung Seong Bae,Damian Chinedu Onwudiwe,Jing Chen,Jun Wu,Wei Lei
Lead halide perovskite single crystals (LHPSC) are promising for room-temperature γ-ray spectroscopy in radiation detection. While MA(CH3NH3)-based LHPSCs are the most straightforward and cost-effective to synthesize from solution, their performance in γ-ray spectroscopy is hindered by significant noise and ion migration at high bias, which degrades their energy resolution (ER). The work introduced an n-type/intrinsic/n-type photodiode incorporating passivation layers of MA-based LHPSCs, grown through solution-process epitaxial growth. This single-polarity device demonstrated an outstanding ER of 3.6% for 662 keV γ-ray photons. Overall, this work provides useful information for developing room-temperature γ-ray detectors based on solution-processed lead halide perovskites.
研究领域:
材料科学
·
辐射探测技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Sustainability
·
2021
·Vol. 5
·期 3
·205-213
·
IF 19.346
Han Daliang,Cui Changjun,Zhang Kangyu,Wang Zhenxing,Gao Jiachen,Guo Yong,Zhang Zhicheng,Wu Shichao,Yin Lichang,Weng Zhe,Kang Feiyu,Yang Quan-Hong
Aqueous zinc (Zn) batteries have long been considered a potentially more sustainable alternative to lithium-ion batteries because of their better environmental compatibility, enhanced safety and cost advantage. However, in the presence of an aqueous electrolyte, the Zn anode is poised to undergo dendrite failure, corrosion and hydrogen evolution, all of which resonate with each other leading to fast performance degradation. Here, in a break from the current aqueous battery path, we report a low-cost hydrous organic electrolyte involving a hydrated Zn(BF 4 ) 2 salt and an ethylene glycol solvent, which not only promotes the in situ formation of a favourable ZnF 2 passivation layer to protect Zn from dendrite growth and side reactions but also embraces excellent non-flammability. Remarkably, the present Zn anode sustains a long-term cycling over 4,000 h at a current density of 0.5 mA cm −2 with a high Coulombic efficiency of 99.4% and shows an areal capacity as high as 5 mAh cm − 2 . Equally intriguingly, the electrolyte can run across a wide temperature range from −30 °C to 40 °C without seriously compromising performance. The Zn//V 2 O 5 full cells with our electrolyte also perform much better in terms of capacity retention than a device with an aqueous ZnSO 4 electrolyte. Our findings suggest a promising direction for developing electrolyte solutions for practical Zn batteries which combine safety, performance and sustainability.
研究领域:
材料科学
·
能源研究
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 41
·19642-19650
·
IF 3.5
Chu Yican,Yao Zhendong,Liu Min,Li Wenqing,Gu Jing,Huang Zhenguang,Xie Jiaxing,Li Chao,Cui Yongfu,Li Yun,Fan Meiqiang
The hydrolysis of silicon and its compounds to produce hydrogen for fuel cell remains a major problem. The main obstacle is the weak hydrolytic activity and slow kinetics of silicon. In this work, the alloying properties of Si and Ca to improve its hydrolytic activity, and studied the film breaking effect of different metals and halogen ions on its passivation layer. The results show that the hydrogen production of the alloy is still determined by its phase composition. Among the common metal (Ni, Bi, Sn) and halogen ions (F – , Cl – ) catalyzed by hydrolysis, Ni and F – showed a good synergistic effect, resulting in a hydrogen yield of 269 mL/g at room temperature without alkali. Graphical
The effects of metal ions and halogens on the hydrolytic properties of Ca–Si alloy were investigated, and Ni 2+ and F — showed good synergistic effect.
研究领域:
材料化学
·
能源材料
·
无机化学
·
氢能源
·
金属合金
✓ 已验证
DOI
高影响因子
VACUUM
·
2023
·
IF 4
Fengquan She,Aosong Gao,Pengfeng Jiang,Yifan Zhou,Xiaoqi Zhang,Muzi Yang,Li Gong,Jian Chen,Xia Lu,Fangyan Xie
The energy density of solid-state lithium metal battery has been greatly improved if it employs lithium metal as the anode because it has high theoretical capacity and most negative electrode potential. However, the highly active surface of lithium metal is usually covered by a passivation layer, which can not be completely removed by conventional methods and greatly affects the performance and safety of the corresponding battery. The existence of the passivation layer is a common sense, but still lacks detailed characterizations, and the researchers rarely focus on lithium metal under the passivation layer. In this work, we use X-ray photoelectron spectroscopy (XPS) to analyze the composition and thickness of the passivation layer to account for the stability of Li metal surface , the results of different pretreatment methods are systematically compared. The parameters used for fitting the XPS results of Li surface are summarized, and the relevant results can be used to compare the general proportion of each component on the surface conveniently and quickly. With argon ion sputtering, we can successfully remove the passivation layer and obtain a clean and fresh surface. With this fresh Li, a symmetric cell is built for electrochemical tests, where it is found significant decrease on the interfacial resistance between the clean lithium metal electrode and the electrolyte with regard to that in the un-treated lithium metal based one. This work opens a rewarding avenue towards the accurate application of XPS to elucidate the specific role of Li metal in stabilizing the interface of solid-state batteries.
研究领域:
材料科学
·
能源存储技术
·
表面分析技术
✓ 已验证
DOI
高影响因子
ACS Nano
·
2025
·
IF 16
Guangwen Zhang,Deyuan Li,Dongfang Yu,Ao Du,Zihui Chen,Huilin Ge,Weiqi Hou,Yizhou Zhu,Chunpeng Yang
Halide solid-state electrolytes (SSEs) with high ionic conductivity and high-voltage stability have attracted significant interest for application in all-solid-state batteries. However, they are not chemically stable against the lithium (Li) metal anode due to continuous side reduction reactions, hindering the application of halide SSEs in high-energy-density all-solid-state Li metal batteries (ASSLMBs). Here, we report a self-limiting layer (SLL) composed of InF3 and Li2ZrCl6 (LZC) to stabilize the halide SSEs and Li metal anode interface, where the in situ generated LiF-rich layer serves as a passivation layer to suppress ensuing reactions and kinetically stabilize the interface between LZC and Li metal anode. As a result, Li metal symmetric cells with LZC protected by the SLL exhibit excellent cycling performance for over 3000 h. The ASSLMBs with SLL achieve 99.2% capacity retention over 100 cycles at 0.5 C and 83.5% capacity retention after 250 cycles at 2 C. Density functional theory-computed thermodynamic data and postcycling experimental characterizations confirm the forming of a LiF-rich passivation layer between the SLL and the Li anode, which effectively prevents continuous side reactions. This self-limiting interface protection offers a feasible kinetical passivation strategy for halide SSEs and the Li metal anode toward high-performance ASSLMBs.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nanomaterials
·
2020
·Vol. 10
·期 4
·631
·
IF 4.324
Zhen Li,Libo Yu,Hao Wang,Huiwen Yang,Huan Ma
Light harvesting and electron recombination are essential factors that influence photovoltaic performance of quantum dots sensitized solar cells (QDSSCs). ZnO hollow microspheres (HMS) as architectures in QDSSCs are beneficial in improving light scattering, facilitating the enhancement of light harvesting efficiency. However, this advantage is greatly weakened by defects located at the surface of ZnO HMS. Therefore, we prepared a composite hollow microsphere structure consisting of ZnO HMS coated by TiO2layer that is obtained by immersing ZnO HMS architectures in TiCl4aqueous solution. This TiO2-passivated ZnO HMS architecture is designed to yield good light harvesting, reduced charge recombination, and longer electron lifetime. As a result, the power conversion efficiency (PCE) of QDSSC reaches to 3.16% with an optimal thickness of TiO2passivation layer, which is much higher when compared to 1.54% for QDSSC based on bare ZnO HMS.Keywords:TiO2passivation layer;ZnO hollow microspheres;quantum dots sensitized solar cells
研究领域:
材料科学
·
能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Physica Status Solidi-Rapid Research Letters
·
2022
·Vol. 17
·期 1
·2200295
·
IF 3.277
Pengpeng Cheng,Zehan Liu,Ruyan Kang,Jian Zhou,Jia Zhao,Zhiyuan Zuo
Perovskite light-emitting diodes (PeLEDs) are generally fabricated in a sandwiched device structure that contains a perovskite emissive layer between the electron transport layer (ETL) and the hole transport layer (HTL). However, protective atmosphere environments are avoidless during the fabrication processes of PeLEDs. Taking the large-scale industrial production into consideration, all-solution method-processed ETL-free PeLEDs under ambient conditions are still highly demanding. This work successfully demonstrates the optimization of blocking passivation layer ETL-free PeLEDs by the all-solution method for manufacturing in ambient conditions. The obtained PeLEDs have a luminance of more than 8200 cd m −2 , which is more than 40 times higher compared with the control device. The optimization mechanism of passivation and synergism effects is proposed. These advances can provide an opportunity to fabricate high-performance perovskite-based photovoltaic devices under ambient conditions.
研究领域:
材料科学
·
光电子学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）