CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Huanwei Shen,Xiayue Yang,Wenhao Li,Zhihua Sha,Hongmei Luo,Zixuan Li,Sihan Dong,Wei Cui,Rong Ran
Improving the evaporation efficiency of solar-driven hydrogel evaporators is crucial for addressing water scarcity. Traditional efforts have been focused on increasing the intermediate water content or shortening the evaporation route through hydrogel structure design. However, rare attempts have been made to combine these two approaches. Here, we report the simultaneous achievement of high intermediate water content and short water transport paths in a hydrogel for efficient solar-driven evaporation. By introducing pullulan and MXene nanosheets into a poly(vinyl alcohol) (PVA) system that is subjected to directional freezing-assisted salting-out, we achieve a considerably high intermediate water to free water ratio of 2.11. Meanwhile, low- tortuosity yet compact channels within the hydrogel formed during directional freezing-assisted salting-out accelerate water transport during evaporation. Consequently, the hydrogel evaporator achieves an energy conversion efficiency of 93 % under one sun illumination, with a high vapor generation rate of 3.92kg m −2 h −1 . Even in highly saline water, an evaporation rate of 2.93 kg m −2 h −1 is preserved, accompanied by voltage generation through water-driven ion migration. Moreover, the hydrogel evaporator can be recycled by heating using the remoulade properties of PVA without deteriorating the evaporation rate, holding great potential in sustainable and recyclable water collection.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Laser & Photonics Reviews
·
2025
·
IF 10
Yuhan Yang,Yang Lu,Yulei Chang,Qiqing Li,Ting Liu,Yuyao Hong,Rui Li,Xu Yan,Peng Sun,Xiaomin Liu,Geyu Lu
Multipolar resonance and cross-relaxation (CR) are the primary mechanisms of non-radiative energy transfer between rare-earth ions. It is well established that upconversion luminescence is enhanced by suppressing CR-mediated depopulation of high-energy levels through cryogenic fields. However, the role of intermediate-state population processes, particularly those dominated by multipolar resonance, has largely been overlooked. In this study, theoretical derivations and experimental results are combined to distinguish, for the first time, between two types of resonance transfer processes: phonon-releasing transfer (RRT) and phonon-absorbing transfer (ART), and their distinct sensitivities to low temperatures are investigated. In both co-doped and Er 3+ -self-sensitized systems, it is demonstrated that the RRT-mediated intermediate state population process is the key factor in the cryogenic enhancement and modulation of luminescence rather than merely the inhibition of CR. Based on these findings, a novel phenomenon of wavelength-dependent, orthogonal temperature-responsive behavior is reported. This study challenges the current consensus and provides new insights into traditional energy transfer mechanisms.
研究领域:
光学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF CHEMICAL PHYSICS
·
2019
·Vol. 151
·期 24
·
IF 2.997
Liu Miao,Fu Qinqin,Wang Xueliang,Xie Degang,Wang Yaping
Understanding the melting behavior of metals at the microlevel and atomic level has been experimentally challenging due to the involvement of multiple phases at ultrafast time scale. By using the confocal scanning laser high-temperature microscope, differential scanning calorimetry, and environmental transmission electron microscope, we observed the transient process during melting of silver (Ag) nanoparticles below the equilibrium melting point. The melting point of Ag nanoparticles with the diameter of 60–120 nm is found to decrease by 100–400 °C, and the melting process is accompanied by a geometrical transformation at 840 °C, from an irregular polyhedron to a nearly spherical crystallinelike liquid with smooth facets. These results indicate that the melting of metal nanoparticles is not a direct sharp transformation from crystal to liquid but a gradual process via a certain intermediate state.
研究领域:
材料科学
·
物理化学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Wen Qin,Chengyuan Zheng,Haoming Qin,Yang Song,Yang Zhou,Jin Jiang,Jun Ma
Permanganate/electron shuttle systems for the enhanced transformation of anilines were evaluated. The presence of electron shuttles (2,2’-azino-bis(3-ethylbenzothiazoline)-6-sulfonate (ABTS), 1-hydroxybenzotriazole (HBT) and catechol (CAT) accelerated the oxidative transformation of aniline by Mn(VII). In the Mn(VII)/ABTS process, ABTS •+ was partially consumed through fragmentation or polymerization with aniline, while the second-order rate constants ( k app 2 , M −1 s −1 ) of the interaction of ABTS •+ with aniline rose from 86.57 to 140.04 M −1 s −1 with increase in pH from 5 to 8. In the Mn(VII)/HBT system, aniline removal was markedly enhanced under acidic conditions due to the formation of polymerized products via radical cations (HBT • ). Furthermore, the oxidative transformation of aniline (82.5 %) by Mn(VII)/CAT was significantly higher than that by Mn(VII) (65.2 %) because of Michael addition reaction of aniline and ortho-benzoquinone (o-BQ). Moreover, the formation of Mn(III) was confirmed by the overall oxidation state (3.13) and the X-ray Photoelectron Spectroscopy (XPS) spectra of the Mn products in the CAT/Mn(VII) process, revealing a synergistic mechanism between o-BQ and Mn(III) for enhanced aniline degradation.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
BIOTECHNOLOGY AND BIOENGINEERING
·
2023
·Vol. 121
·期 3
·1005-1015
·
IF 3.8
Xiaomin Yi,Hongwei Yu,Lidan Ye
Bioproduction of chiral amines is limited by low transaminase (TA) activity on nonnatural substrates, leading to the need for protein engineering. To address the challenge of quickly and precisely identifying the engineering targets, a strategy was proposed based on analyzing the mode changes in the high-energy intermediate state (H-state) of the substrate–enzyme complex during catalysis. By substituting the residues with minimal structural changes in catalytically active mode (A-mode) and distance-free mode (F-mode) of the H-state complex with more conserved ones to stabilize it, a TA mutant M5(T295C/L387A/V436A) with 121.9-fold higher activity for synthesizing the ( S )-Rivastigmine precursor ( S )-1-(3-methoxyphenyl)ethylamine was created. The applicability of this strategy was also validated by engineering another TA for 1.52-fold higher activity and >99% selectivity toward ( R )-3-amino-1-butanol biopreparation. The much higher stereoselectivity of the mutant compared with the wild type (28.3%) demonstrated that this strategy is not only advantageous in engineering enzyme activity but also applicable for modulating stereoselectivity.
研究领域:
生物化学
·
蛋白质工程
·
酶学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Science
·
2020
·Vol. 7
·期 5
·1903009
·
IF 15.84
Shubo Wang,Yiqi Chen,Ruiyi Li,Yibo Xu,Jiangshan Feng,Dong Yang,Ningyi Yuan,Wen-Hua Zhang,Shengzhong (Frank) Liu,Jianning Ding
As the power conversion efficiency (PCE) of perovskite solar cells (PSCs) is increased to as high over 25%, it becomes pre-eminent to study a scalable process with wide processing window to fabricate large-area uniform perovskite films with good light-trapping performance. A stable and uniform intermediate-state complex film is obtained by using tetramethylene sulfoxide (TMSO), which extends the annealing window to as long as 20 min, promotes the formation of a high-quality perovskite film with larger grains (over 400 nm) and spontaneously forms the surface texture to result in an improved fill factor and open-circuit voltage ( V oc ). Moreover, the superior surface texture significantly increases the long-wavelength response, leading to an improved short-circuit current density ( J sc ). As a result, the maximum PCE of 21.14% is achieved based on a simple planar cell structure without any interface passivation. Moreover, a large area module with active area of 6.75 cm 2 is assembled using the optimized TMSO process, showing efficiency as high as 16.57%. The study paves the way to the rational design of highly efficient PSCs for potential scaled-up production.
研究领域:
材料科学
·
能源技术
✓ 已验证
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2023
·
IF 6.2
Hong Sun,Chuan Yao,Kaibo You,Can Chen,Shuoshuo Liu,Zhihong Xu
Unclear issues in protein studies include but not limited to the stability and denaturation mechanism in the presence of denaturants. Herein, we report a dynamic monitoring approach based on nanopore single-molecule biosensor , which can detect the protein's folding and unfolding transitions by recording a nanopore ionic current . When gradually increasing the concentration of denaturant guanidine hydrochloride (GdmCl), sensitive responses were observed with lysozyme unfolding. The emergence of the featured biphasic-pulse demonstrated the existence of a stable intermediate. It was the first time to experimentally confirm the dynamic equilibrium between the intermediate and the native states at single molecule level, therefore consolidating the standpoint of lysozyme denaturation process following the three-state model. Additionally, we got more insights into the conformation about the intermediate as globular-like structure, larger gyration radius, and enhanced positive charge density. We considered that the manner of denaturant toward lysozyme adopts the “direct” model based on stronger electrostatic and van der Waals forces . Nanopore biosensor exhibited excellent sensitivity with a low detection concentration of 280 pM and reproducibility in analysing the folding intermediate of lysozyme.
研究领域:
生物物理学
·
分子生物学
·
生物化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Meng Yang,Heng Luo,Weizhi Zou,Yong Liu,Jinhao Xu,Jing Guo,Jian Xu,Ning Zhao
Optimizing the water bonding network in an evaporator is significant for efficient solar-driven vapor generation (SVG). Herein, we report a facile one-pot method to regulate the hydrated structure and wettability in a hierarchical porous hydrogel. An ovalbumin (OVA)-polyacrylamide hydrogel foam was fabricated in a cake-making fashion. Because of the enrichment of amphiphilic OVA at the interface, the hydrophobic walls of the air pores in the foam provide vaporization sites and help reduce parasitic heat loss, while the hydrophilic skeleton with the secondary pores effectively pumps capillary water. Notably, the proportion of intermediate water in the foam reaches 87.6% with the melting point as low as −10 °C. All these features contribute to an exceptional evaporation rate of 3.4–4.5 kg m–2 h–1 under 1 sun and robust SVG performances at high-humidity, weak sunlight, or cold weathers. The strategy of using amphiphilic molecules to optimize the hydrated structures both at the interface and in bulk promises the reasonable design of SVG materials with superior efficiency and weather adaptability.
研究领域:
材料科学
·
能源科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Qin Guo,Ying Cao,Jin Jiang,Juan Li
The permanganate/sulfite (Mn(VII)/sulfite) process has shown promise for degrading recalcitrant organic micropollutants, yet current methods to differentiate the roles of intermediate manganese species (IMS) and sulfate radicals (SO₄ •- ) show limitations. In this study, atrazine (ATZ) - a widely detected and oxidation-resistant herbicide - was used as a probe compound to investigate the reactivity of IMS and SO₄ •- generated in the Mn(VII)/sulfite system. ATZ exhibited negligible degradation by Mn(VII) alone but underwent rapid transformation within seconds in the presence of sulfite, with degradation efficiency increasing at lower pH and optimal [Mn(VII)]/[sulfite] ratios. Using stopped-flow spectrophotometry, pseudo-first-order kinetics were confirmed. Six major transformation products were identified, among which atrazine amide (CDIT) and desethyl-atrazine (DEA) were predominant. The molar ratio of CDIT to DEA ([CDIT]/[DEA]) was evaluated as a mechanistic indicator. A consistent ratio of ~4.8 at low sulfite levels indicated Mn(V)-dominated oxidation, while lower ratios at higher sulfite concentrations reflected increasing contributions from Mn(III) and SO 4 •− . This trend was supported across pH 3, 5, and 7. Water matrix components such as natural organic matter and nitrite were found to inhibit ATZ degradation, likely due to their scavenging of reactive species. This study establishes the [CDIT]/[DEA] ratio as a novel mechanistic indicator in manganese-activated oxidation and highlights the Mn(VII)/sulfite process as an effective strategy for degrading recalcitrant micropollutants in water treatment.
研究领域:
环境化学
·
水处理技术
·
氧化还原过程
·
污染物降解机制
·
自由基化学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2025
·
IF 26.8
Meng Cai,Wei Liu,Tiankai Zhang,Pengfei Yan,Yuxuan Li,Weiqian Kong,Hangjuan Wu,Zongwei Chen,Zhenkun Gu,Lin Dong,Qun Xu,Yanlin Song,Junjie Ma,Chongxin Shan,Feng Gao
All-inorganic CsPbX 3 (X = I, Br, Cl) perovskites emerged as a crucial material for addressing the stability bottleneck due to their exceptional resistance to both light-thermal stress. However, their performance is limited by adverse optoelectronic dissipation arising from inadequate photon conversion and chaotic carrier energetics. Herein, the mechanism of the unique nonlinear plasmonic effect in van der Waals 2D MoO 3-x is elucidated, which is mediated by electronic intermediate states. It demonstrates that the 2D MoO 3-x serves as a light-capture-antenna in heterodimensional CsPbX 3 -MoO 3-x optically coupled system, contributing to the accumulation the optical field energy on the nanoscale and resulting in a remarkable 59% increase in photon convergence. Additionally, facet-oriented carrier channels can be established through heteroepitaxy along matched Mo-O octahedron. This optoelectrical-bimodal-coupling engineering combined with a bifacial light-harvesting configuration yields a bifacial equivalent efficiency of 27.33%, which stands as the supreme performance in all-inorganic perovskite photovoltaics. Graphical This remarkable work combines supercritical CO 2 chemical engineering, two-dimension plasmon photophysical science, and perovskite photovoltaic technology. It introduces novel concepts like broad - spectrum coupled photon absorption, the intermediate - localized - states model, and optoelectrical - bimodal - coupling engineering. It aims to combat optoelectronic dissipation and enhance energy harvesting via a heterodimensional van der Waals optically coupled system.
研究领域:
光伏技术
·
等离激元学
·
纳米光子学
·
材料科学
·
光电子学
·
钙钛矿太阳能电池
·
固体物理学
✓ 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）