Energy & Environmental Science
·
2024
·
IF 32.4
Cong Liu,Anweng Gong,Chen Zuo,Tao Liu,Xiaoyang Liang,Donglou Ren,Kai Shen,Jianzha Zheng,Qifan Xue,Zhiqiang Li,Ruud E. I. Schropp,Bingsuo Zou,Yaohua Mai
High-quality heterojunctions are crucial for achieving high power conversion efficiency (PCE) in the antimony selenosulfide (Sb2(S,Se)3) solar cells. Here, we introduce lithium fluoride (LiF) doping of the precursor solution to improve the conductivity, morphology, and n-type characteristics of cadmium sulfide (CdS) films. In addition, Li-ions have high mobility, which enhances in situ diffusion into the Sb2(S,Se)3 absorber layer during subsequent hydrothermal deposition. Li effectively passivates selenium vacancies (VSe) and antimony anti-site (SbS) defects through the formation of Li–S(e) bonds. This lithiation process not only realizes a twofold optimization of the CdS buffer layer and the Sb2(S,Se)3 absorber layer, but also yields a favorable energy level arrangement and a wider depletion region at the CdS/Sb2(S,Se)3 heterojunction. By this way, we have achieved a champion PCE of 10.76% compared to a certified value of 10.50% for Sb2(S,Se)3 solar cells, which is the highest certified efficiency reported for Sb-based solar cells so far. This study provides a convenient method to optimize dual functional layers and heterojunctions for high-performance Sb2(S,Se)3 solar cells.
研究领域:
材料科学
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能源科学
·
光伏技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Physical Chemistry Letters
·
2022
·
IF 6.888
Zejian Dong,Na Zhang,Shuangbao Wang,Yuying Liu,Lifeng Zhang,Xing Chen,Langli Luo
Atomic defects are critical to tuning the physical and chemical properties of functional materials such as catalysts, semiconductors, and 2D materials. However, direct structural characterization of atomic defects, especially their formation and annihilation under practical conditions, is challenging yet crucial to understanding the underlying mechanisms driving defect dynamics, which remain mostly elusive. Here, through in situ atomic imaging by an aberration-corrected environmental transmission electron microscope (AC-ETEM), we directly visualize the formation and annihilation mechanism of planar defects in monoclinic WO3 on the atomic scale in real time. We captured the atomistic process of the nucleation dynamics of the dislocation core in the [010] direction, followed by its propagation to form a planar defect. Corroborated by density functional theory-based calculations, we rationalize the formation of dislocation through O extraction from bridge sites followed by an atomic channeling process. These in situ observations shed light on the defect dynamics in oxides and provide atomic insights into forming and manipulating defects in functional materials.
研究领域:
材料科学
·
纳米技术
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凝聚态物理
·
催化
·
显微学
✓ 已验证
DOI
高影响因子
Journal of Physical Chemistry C
·
2022
·
IF 4.177
Hang Mei,Zi-Yan Wang,Yue Zhai,Qiang-Qiang Zhu,Le Wang,Pei Liang
Vacancy-ordered double perovskites, the variant of metal-halide perovskites, have excellent potential for use in optoelectronic and thermoelectric devices. A narrow region of forming the stable vacancy-ordered double perovskite Cs2PdBr6 by the chemical potential calculation via the first principles method was reported. Perdew–Burke–Ernzerhof functionals were used to investigate the possible intrinsic defects and the corresponding formation energy of Cs2PdBr6. Under the Pd-rich condition, the VBr defect was spontaneously formed as it has the lowest formation energy among all donor defects. In contrast, the sample became a p-type conducting material with a high hole concentration under the Pd-poor condition. This indicates that the defect-induced decline of photoelectric properties of Cs2PdBr6 can be alleviated by regulating the VBr defect alone. Finally, the Cs2PdBr6 microcrystals were fabricated via hydrothermal synthesis. In addition, XRD, PL, and Raman spectroscopy were also performed on Cs2PdBr6 powder to characterize the microstructure and optical properties of the compound; the results showed that VBr defects can be formed spontaneously, which is consistent with our theoretical calculations.
研究领域:
材料科学
·
物理化学
✓ 已验证
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Shuaichuan Cui,Xingxing Wang,Yifan Huang,Shihan Liu,Ziming Li,Yifan Zhang,Shusen Chen,Pengyang Deng
Herein, a defect-rich UiO-66-NH 2 hybrid membrane (DUUM) was successfully synthesized via in-situ growth of defective UiO-66-NH 2 onto irradiation-treated ultra-high molecular weight polyethylene fabrics to enhance the uranium extraction from seawater. The concentration of lattice defects within the framework is regulated by simply adjusting the ratio of ligand to metal (L/M), and DUUM with the L/M ratio of 1 exhibits the best uranium adsorption capacity. The adsorption kinetics investigation shows that DUUM has a higher adsorption rate than UiO-66-NH 2 powders, and the adsorption isotherms investigation shows DUUM has a saturated uranium adsorption capacity of 460 mg·g −1 which is about 5 times that of the defective UiO-66-NH 2 powders. DUUM exhibits a flux of 1440 LMH and a uranium removal efficiency of 65.5 % from natural seawater through single-pass filtration. More importantly, DUUM demonstrates excellent stability in real seawater environments (40-day) and under high doses of gamma-ray irradiation (300 kGy). The enhanced adsorption capacity is attributed to the membrane structure of DUUM which enhances exchange efficiency at the interface between uranium and DUUM via filtration, and the lattice defects which increase the specific surface area and expose more adsorption sites. The high stability results from the inherent hydrophobicity and radiation crosslinking features of the UP substrates. This study about DUUM will promote the practical application of efficient MOF membrane in fast uranium extraction from real seawater, as well as nuclear wastewater.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2024
·
IF 4.3
Cong Xiang,Jingyi Fang,Yanlin Huang,Zhuo Zheng,Hyo Jin Seo
Eu 3+ is not only a major red-emitting activator, but also an excellent spectral probe ion. This work reports the Eu 3+ -sites and luminescence in the cation-deficient perovskite tungstates, A-site deficient SrLa 2 (Mg 2 W 2 )O 12 [Sr 1/2 □ 1/2 La(MgW)O 6 ] and B-site deficient Sr 2 La 2 (MgW 2 )O 12 [SrLa(Mg 1/2 □ 1/2 W)O 6 ]. The 7 F 0 → 5 D 0 excitation spectra of Eu 3+ activators in two lattices were measured via pulsed dye laser. In SrLa 2 (Mg 2 W 2 )O 12 :Eu 3+ , there is only one 7 F 0 → 5 D 0 transition, which could be related to the Eu 3+ center on La 3+ sites; while, two 7 F 0 → 5 D 0 transitions in Sr 2 La 2 (MgW 2 )O 12 indicate Eu 3+ ions occupy Sr 2+ in addition to La 3+ , resulting in the luminescent centers related to heterovalent substitution defects. The different Eu 3+ sites make two phosphors exhibit different red luminescence properties. SrLa 2 (Mg 2 W 2 )O 12 :Eu 3+ shows higher luminescent efficiency and thermal quenching due to its regular distribution of the activators resulting in lower dispersion losses of the energy transfer. The experimental results show that rare earth ions occupy different crystallographic positions in A -site and B -site deficient perovskite oxides, and this microstructure can be important for the corresponding luminescent properties.
研究领域:
材料科学
·
光学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Na Zhou,Jiazhi Wang,Ning Zhang,Zhi Wang,Hengguo Wang,Gang Huang,Di Bao,Haixia Zhong,Xinbo Zhang
Electrochemical conversion of nitrate (NO 3 − ) pollutants into chemical feedstock and fuel ammonia (NH 3 ) can contribute to sustainable mitigation of the current severe energy and environmental crises. However, the electrocatalytic NO 3 − reduction to NH 3 (NRA) involves a sluggish multielectron and proton transfer process that competes with the hydrogen evolution reaction (HER) in aqueous media, imposing great challenges in developing highly selective catalysts for NRA. In this study, we developed a copper and copper-tetracyanoquinodimethane composite catalyst (Cu@CuTCNQ), which possesses a high density of copper vacancy defects. This catalyst has been proven to be efficient for NRA through an in situ electrochemical reconstruction method. The structural evolution of CuTCNQ during NRA was investigated by in situ Raman spectroscopy, which indicated an accelerated charge transfer from the CuTCNQ substrate to the derived Cu, which facilitated the adsorption activation of NO 3 − . The obtained Cu@CuTCNQ exhibited an excellent catalytic performance for NRA, with a Faradaic efficiency of 96.4% and productivity of 144.8 μmol h −1 cm −2 at −0.6 V vs . a reversible hydrogen electrode, superior to Cu nanoparticle counterparts and most Cu-based catalysts. Cu vacancy defects and sufficient interfacial charge transfer synergistically optimize the charge distribution of Cu active sites, reduce the energy barrier for NO 3 − adsorption, and promote deoxidation and hydrogenation processes, thus enhancing NRA and selectivity.
研究领域:
材料科学
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环境科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
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IF 6.3
Junzhou Men,Yi Zheng,Chen Luo,Hui Xian,Yuxia Zhang,Yating Wang,Tao Jiang
Defect engineering is crucial for optimizing the band structures and charge separation of photocatalysts. Herein, the quantity and distribution (core/shell) of organic ligand defects in leaf-shaped zeolite imidazole framework (ZIF-L) composites were modulated via a multi-step method. VZ-12@ZIF-L (with 12 % 1-vinylimidazole in the core) exhibited the highest carrier separation efficiency and the strongest driving force for the hydrogen evolution reaction (HER), achieving a hydrogen evolution rate of 443.19 μmol·h⁻¹ ·g⁻¹ . This rate is 1.81 times that of VZ-25@ZIF-L (with a high defect quantity) and 1.40 times that of ZIF-L@VZ-12 (with defects in the shell). Mechanistically, core defects facilitated the transport of photogenerated carriers, while shell defects narrowed the band gap. Notably, the impact of carrier transport capacity on photocatalytic activity was more significant than that of light absorption. This study provides new insights for the design of efficient defect-engineered metal-organic frameworks (MOFs).
研究领域:
材料科学
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光催化
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金属有机框架
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能源化学
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纳米材料
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半导体物理
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表面科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Nano
·
2025
·
IF 16
Xuan Cao,Wei Mao,Yingze Song,Shaochun Tang
Most current regeneration methods are predicated on the assumption of uniform degradation, making them inadequate to precisely address the structural disparities and defect heterogeneity among particles, thereby limiting their applicability for large-scale regeneration of industrial LiFePO4 black mass. In this work, we propose a scalable and simplified solid–liquid hybrid strategy that enables efficient regeneration of kilogram-scale, heterogeneously degraded LiFePO4 cathodes at room temperature under laboratory conditions. The approach leverages localized interfacial redox processes at room temperature to achieve precise lithium compensation at the particle level. However, atomic-resolution analyses reveal that lithium replenishment alone is insufficient to repair Fe/Li antisite defects within the crystal lattice, particularly in mildly delithiated particles (<5%), where the migration energy barrier reaches 2.78 eV, thus impeding deep structural recovery. To overcome this limitation, a subsequent thermal activation step is incorporated to eliminate deep-seated antisite defects and enable complete lattice reconstruction. This combined approach leads to multiscale structural recovery, allowing the regenerated material to achieve a reversible specific capacity of 114.2 mA h g–1 at 10.0 C and retain 79.2% of its capacity after 1500 cycles. These findings validate the method’s wide applicability to structurally complex degradation scenarios and offer mechanistic and practical insights into scalable regeneration of high-performance electrodes.
研究领域:
材料科学
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电化学
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能源存储
·
再生技术
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纳米材料
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固态化学
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电池回收
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nano Research
·
2023
·Vol. 17
·期 1
·297-306
·
IF 9.9
Xie Jing,Lu Zhenjiang,Feng Yue,Huang Jianguo,Hu Jindou,Hao Aize,Cao Yali
Defect modulation currently plays a decisive role in addressing the poor photoabsorption, sluggish electron hole separation, and high CO 2 activation barrier in photocatalytic CO 2 reduction. However, hunting for a straightforward strategy to balance the concentration of oxygen vacancy and metal cation defect in one photocatalyst is still a great challenge. Herein, a bismuth vacancies BiOBr nanosheets (BiOBr-1) on the exposed [001] facets were constructed via an acetic acid molecule modification strategy, which can repair oxygen defect by bismuth vacancy in low-temperature solid-state chemical method. Benefiting from the formed bismuth defects that can not only broaden light absorption and elevate charge separation efficiency, but also enhance adsorption and activation of CO 2 molecules, the evolution rates of photocatalytic CO 2 conversion into CO (71.23 µmol·g −1 ·h −1 ) and CH 4 (8.90 µmol·g −1 ·h −1 ) attained by BiOBr-1 are superior 7.1 and 11 times to that of plate-like BiOBr. The photocatalytic mechanisms including adsorption concentration and activation process of CO 2 are further revealed by the in situ diffuse reflectance infrared flourier transform spectra (DRIFTS). This finding of the existence of distinct defects in ultrathin nanosheets undoubtedly leads to new possibilities for photocatalyst design using two-dimensional materials with high solar-driven photocatalytic activity.
研究领域:
材料科学
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环境科学
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纳米技术
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催化
·
物理化学
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2022
·
IF 5.532
Wei Zhou,Minghe Cao,Hongye Wang,Hua Hao,Zhonghua Yao,Hanxing Liu
The miniaturization of electronic components requires materials with colossal permittivity. In this work, titanium-powder-doped TiO 2 ceramics with colossal permittivity and a low dielectric loss over a wide range of frequency and temperature were successfully prepared using a solid-state reaction in an Ar atmosphere. TiO 2 ceramics with 2% Ti powder doping had the highest permittivity (110,000) and the lowest dielectric loss (0.029) at 1 kHz and room temperature. Systematic defect analysis showed that Ti 4+ was successfully reduced to Ti 3+ through doping with Ti metal powder. Further, oxygen vacancies were created in the high-temperature inert atmosphere, which promoted the formation of defect clusters with T i 3 + − V o ″ − T i 3 + as the core. Polarization and local confinement of the defect clusters resulted in the colossal permittivity and low dielectric loss. Therefore, this work provides necessary information and novel ideas for the design of correlated defects in colossal permittivity materials.
研究领域:
材料科学
·
电气工程
·
陶瓷
·
缺陷工程
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2021
·Vol. 13
·期 16
·7801-7809
·
IF 7.79
Wanguo Gao,Xiaoman Li,Xu Zhang,Senda Su,Shijian Luo,Rong Huang,Yuan Jing,Min Luo
The vacancies of semiconductors have proven to be effective active sites for photocatalytic nitrogen fixation, but what about the role of defects in MOF materials? Herein, we report the first UiO-66 with photo-excited cluster defects and linker defects for photocatalytic nitrogen fixation. It was determined through the post-synthetic ligand exchange (PSE) process that the linker defects, rather than cluster defects, can greatly improve the performance, which is due to linker defects forming unsaturated metal nodes such as the vacancy in a semiconductor. Specifically, for photo-activated UiO-66, the NH4+ production rate was 196 and 68 μmol g−1 h−1 in air atmosphere under ultraviolet-visible (UV-Vis) and visible light, respectively. This report provides a new effective strategy to design efficient nitrogen fixation photocatalysts.
研究领域:
材料科学
·
化学
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2025
·
IF 12.4
Ziyi Zhao,Yanan Mi,Shili Wang,Xuedong Du,Qingrui Zhang
We firstly present a novel strategy for enhancing fluoride removal from contaminated water using defect-engineered UiO-66 (Zr-MOFs), emphasizing the crucial role of pKa in modulator selection. By utilizing modulators with varying pKa values-specifically benzimidazole (BI), benzoic acid (BA), and acetic acid (AA)-we synthesized defect-rich Act-UiO-66-M(X). The higher pKa of BI facilitated greater defect formation, resulting in significantly improved adsorption capacity and faster diffusion rates. Act-UiO-66-BI(8), modulated with BI, showed a higher intensity peak at g = 2.003 in ESR analysis, indicating more oxygen vacancies. Its fluoride adsorption capacity reached 93.59 mg F/g, nearly six times higher than commercial ZrO 2 , with rapid kinetics—evidenced by a kinetic rate constant (k int ) of 2.64 mg/g·min 0.5 and equilibrium achieved within 10 minutes. The kinetic performance was enhanced by 270% compared to raw Act-UiO-66. Furthermore, Act-UiO-66-BI(8) demonstrated high selectivity and stability in high-salinity environments, with a K d coefficient consistently exceeding 17,900 mL/g. The study highlights that selecting modulators based on pKa enhances defect formation, improving active site exposure and pore diffusion, as confirmed by DFT calculations and XPS analysis. The ability of Act-UiO-66-BI(8) to treat up to 1160 kg of wastewater per kg of adsorbent highlights its potential for large-scale water purification, showcasing a promising approach for developing high-performance MOF materials.
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
危险品化学品经营许可证（带存储）