Journal of Physical Chemistry C
·
2022
·
IF 4.177
Zi Yin,Jiangwen Liao,Guikai Zhang,Shouwei Zuo,Shengqi Chu,Lirong Zheng,Pengfei An,Huan Huang,Juncai Dong,Jing Zhang
Surface ligand passivation strategies have been extensively used to produce metal halide perovskite nanoparticles (NPs) with excellent optoelectronic properties, and a better understanding of the ligand–NP interactions is essential to unleash the full potential of perovskite NPs. Here, the well-passivated methyl ammonium lead bromide NPs were obtained when (3-aminopropyl) triethoxysilane (APTES) and oleic acid (OA) were involved as efficient dual surface ligands. We systematically explored ligand–NP interactions by using spectroscopic analysis and theory calculations. Our results demonstrated that –[−OOC–R]− from OA would preferably occupy the Br vacancies on the surface under-coordinated Pb sites in the corner-sharing octahedral framework to form [PbBr5]3–-[−OOC–R]− complexes, whereas –NH3+ of APTES can connect with Br– on the NP surface via hydrogen bonds. These surface binding interactions can trigger the lattice contraction of NPs, which can lead to an increased Pb2+ off-centering by promoting the lone pair stereochemical activity. Furthermore, the electronic band structure can be modulated by orbital interactions within the inorganic Pb–Br frame through the surface ligand effect. This work not only increases our understanding of ligand–NP interactions in terms of coordination geometry but also reveals their influence on the stereochemical activity of the Pb 6s2 electron pair, which will provide valuable inspiration for the ligand passivation strategies in the future.
研究领域:
材料科学
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物理化学
✓ 已验证
产品关联
DOI
高影响因子
Cell Reports Physical Science
·
2023
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IF 8.9
Zheng Hu,Hui Li,Wenbo Zhao,Wei Zhou,Shi Hu
Structural information in a disordered atomic system cannot be acquired from everyday X-ray diffractometers, so we have to resort to synchrotron resources. The pair distribution function from synchrotron X-ray and neutron scattering reflects the local bond information regardless of the crystallinity, but the limited access to these high-energy light resources prevents them from widespread use. Here, we develop a microstructure analysis framework to study immiscible binary alloys through the integration of local elemental segregation analysis, electron-based pair distribution function, the corresponding wavelet coherence spectrum, and ab initio level simulation. All the information can be obtained from an in-house transmission electron microscope equipped with an energy-dispersive spectroscope. A series of nanoparticles based on immiscible Pd-Ru alloys are chosen as model catalysts for the hydrogen evolution reaction, and the structure-performance relationship is established on the basis of the electrochemical tests and structural information from the analysis toolkit we developed.
研究领域:
材料科学
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催化化学
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电子显微学
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DOI
高影响因子
Matter
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2023
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IF 18.9
Wenda Li,Lingyan Huang,Hongyi Zhang,Yong Wu,Facai Wei,Tingting Zhang,Jianwei Fu,Chengbin Jing,Jiangong Cheng,Shaohua Liu
Construction of covalent organic frameworks (COFs) with fine-tuning pore structures and crystalline orientations at the nano-/meso-scale is vital for their potential applications, but common synthesis routes for COFs always result in the unpredictable nucleation growth and aggregation of small crystals with arbitrary orientations and geometries. Here, we develop a supramolecular mineralization strategy for controllable fabrication of semiconducting COF nanoarchitectures by pre-assembly and subsequent in situ covalent locking of supramolecules. This strategy allows us to change the dynamic covalent chemistry reaction path by reducing the entropy of the system, thus facilitating control over the growth and crystallization of COFs on demand (including 1D, 2D, etc.). The tailor-made COF can effectively suppress the shuttle effect and accelerate the conversion of polyiodide through strong intrinsic electron-pair induce interactions, thereby delivering an outstanding performance in zinc-iodine batteries. The studies create a link between supramolecular chemistry and polymer science for the controllable construction of COF and supramolecular materials.
研究领域:
材料化学
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纳米科学
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电化学
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能源存储
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高分子科学
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超分子化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Meichun Fu,Zhiyu Shao,Yuan Zhang,Qian Zhu,Kuo He,Mengzhu Zhang,Yuzhu Hou,Laiping Fang,Fei Yan,Shuang Zhang,Jianshi Du,Ping’an Ma,Keke Huang,Shouhua Feng
Despite the multiple advantages of high tissue penetration depth, selectivity, and noninvasiveness of photothermal-assisted antitumor synergistic therapy, developing photothermal agents with multifunctional characteristics, desirable tumor therapeutic effects, and biological stability remains a key challenge. Herein, an electronic structure-regulated strategy is proposed to activate self-adaptive Sn–Fe electron pair centers (Sn2+/Sn4+ and Fe2+/Fe3+) through loading the electron donor Pt (Pt/SFO-1, -2, -3, -4). Experimental and theoretical calculations indicate that abundant dynamic active centers can facilitate the production of reactive oxygen species (ROS), which enables Pt/SFO samples to possess catalase (CAT), peroxidase (POD), and oxidase (OXD) enzyme-like activities. Upon near-infrared (NIR) laser irradiation, Pt/SFO-2 with a Pt load of 0.9% achieves the highest ROS production, showing a 9-fold compared with SnFe2O4 and implements the synergistic therapy of photothermal therapy (PTT), photodynamic therapy (PDT), and chemodynamic therapy (CDT). The electronic state regulation of inorganic photothermal agents not only improves tumor therapeutic effects but also offers a novel strategy to regulate the electron structure of active centers.
研究领域:
生物医学工程
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材料科学
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肿瘤学
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纳米技术
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无机化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
BIORESOURCE TECHNOLOGY
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2022
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IF 11.889
Lei Yu,Wei-xin Cheng,Quan Wang
Biohydrogen productions from xylose and glucose under dark condition were enhanced by the presence of natural Fe 3 O 4 . The electron equivalent of H 2 fractions accounted for 4.55 % and 5.69 % of the total given xylose and glucose in the experiments without Fe 3 O 4 , and that were correspondingly increased to 5.14 % and 6.50 % in the experiments with 100 mg/L of Fe 3 O 4 , respectively. Moreover, Fe 3 O 4 increased the total intracellular NAD(H) concentrations by 8.84 % and 8.37 %, and boosted the ratios of NADH/NAD + by 8.33 % and 17.72 % in xylose and glucose fermentation, respectively, comparing to the corresponding control experiments. The formation of electron couples of Fe(III)/Fe(II) during the iron oxide respiration and more generation of active extracellular polymeric substances components were determined as the important reasons for the improved biohydrogen production performance. Thus, a promotion mechanism of the internal “driving forces” from extracellular iron oxide respiration on the biohydrogen production was proposed.
研究领域:
生物技术
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环境工程
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微生物学
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产品关联
DOI
PubMed
高影响因子
Advanced Science
·
2022
·Vol. 9
·期 14
·2105787
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IF 17.521
Jindong Chen,Qingchen Wu,Haotian Tian,Xiaotian Jiang,Feng Xu,Xin Zhao,Zheshuai Lin,Min Luo,Ning Ye
Pnictides are superior infrared (IR) nonlinear optical (NLO) material candidates, but the exploration of NLO pnictides is still tardy due to lack of rational material design strategies. An in-depth understanding structure–performance relationship is urgent for designing novel and eminent pnictide NLO materials. Herein, this work unravels a vital band gap mechanism of pnictides, namely P atom with low coordination numbers (2 CN) will cause the decrease of band gap due to the delocalization of non-bonding electron pairs. Accordingly, a general design paradigm for NLO pnictides, ionicity–covalency–metallicity regulation is proposed for designing wide-band gap NLO pnictides with maintained SHG effect. Driven by this idea, millimeter-level crystals of MgSiP2 are synthesized with a wide band gap (2.34 eV), a strong NLO performance (3.5 x AgGaS 2 ), and a wide IR transparency range (0.53–10.3 µm). This work provides an essential guidance for the future design and synthesis of NLO pnictides, and also opens a new perspective at Zintl chemistry important for other material fields.
研究领域:
材料科学
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非线性光学
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固态化学
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津特尔化学
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红外材料
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DOI
高影响因子
Nature Energy
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2022
·Vol. 7
·期 9
·866-875
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IF 67.439
Zhai Shuo,Xie Heping,Cui Peng,Guan Daqin,Wang Jian,Zhao Siyuan,Chen Bin,Song Yufei,Shao Zongping,Ni Meng
Improved, highly active cathode materials are needed to promote the commercialization of ceramic fuel cell technology. However, the conventional trial-and-error process of material design, characterization and testing can make for a long and complex research cycle. Here we demonstrate an experimentally validated machine-learning-driven approach to accelerate the discovery of efficient oxygen reduction electrodes, where the ionic Lewis acid strength (ISA) is introduced as an effective physical descriptor for the oxygen reduction reaction activity of perovskite oxides. Four oxides, screened from 6,871 distinct perovskite compositions, are successfully synthesized and confirmed to have superior activity metrics. Experimental characterization reveals that decreased A-site and increased B-site ISAs in perovskite oxides considerably improve the surface exchange kinetics. Theoretical calculations indicate such improved activity is mainly attributed to the shift of electron pairs caused by polarization distribution of ISAs at sites A and B, which greatly reduces oxygen vacancy formation energy and migration barrier.
研究领域:
材料科学
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化学
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能源技术
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机器学习
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
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2021
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IF 7.086
Yan Cao,Linfeng Zhang,Yingxue Geng,Yingjie Li,Qun Zhao,Jianhong Huang,Ping Ning,Senlin Tian
Polycyclic aromatic hydrocarbons (PAHs) can penetrate and accumulate in the pulmonary surfactant (PS) membranes, leading to abnormalities of biological macromolecules and the destruction of membrane structure and properties. In the present study, the bioavailability , apparent permeability, effective permeability and residual coefficient of 10 PAHs on PS membrane was assessed by the parallel artificial membrane permeability assay (PAMPA). The influence of various forces on permeability is obtained by analyzing the correlation between parameters and physicochemical properties . Research shows that octanol-water partition coefficient ( K ow ) cannot directly predict permeability, and permeability has no significant relationship with polarity. Dispersion, induction, coupling/polarization promote permeation, while hydrogen bonded acid and n-n electron pair inhibit permeation. Further surface pressure-area (π-A) isotherms test and Brewster angle microscope observation manifested that there are huge differences in the transmembrane ability and effects on the membrane of PAHs with different structures. This work has considerable significance that will help to evaluate the bioavailability and human health risk of PAHs.
研究领域:
环境科学
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毒理学
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生物物理学
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化学
✓ 已验证
DOI
高影响因子
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