INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Maohao Yang,Wanyin Ge,Toshiharu Teranishi
Inorganic metal halides (IMHs) often suffer from severe fluorescence thermal quenching, limiting their application at elevated temperatures. Therefore, the exploration of IMHs exhibiting antithermal quenching (ATQ) behavior is of great importance. In this study, we developed a green synthetic route using a solvent evaporation method to successfully synthesize the 0D IMHs Cs2InCl5(H2O). By precise control over the doping ratios of Sb3+, Yb3+, and Er3+, unique dual-mode emission properties are obtained. As the temperature increases, the compound exhibited downconversion and upconversion luminescence, with relative sensitivity SR-max values of 7.11% K–1 and 1.21% K–1, respectively. Particularly anomalous is the compound’s manifestation of an unconventional ATQ behavior during the upconversion process. In situ structural analysis confirmed that under high-temperature conditions, the 0D Cs2InCl5(H2O) metal halide undergoes structural evolution, transitioning through a Cs3In2Cl9 phase, which is responsible for the ATQ. This study provides experimental evidence for the abnormal ATQ of 0D metal halides, offering new inspiration for the multifunctionalization of 0D metal halides in high-temperature temperature sensing and dual-mode luminescence.
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DOI
PubMed
高影响因子
Advanced Optical Materials
·
2024
·Vol. 12
·期 20
·2400184
·
IF 8
Yue Li,Haolin Lu,Rui Yun,Huanxin Yang,Yuling Liu,Zhaoyu Wang,Song Wang,Guankui Long,Xiyan Li
Lead-free perovskites exhibit unique crystal structures and optical properties due to their low-dimensional structure. However, the 0D structure of Cs 2 InCl 5 ·H 2 O usually demonstrates poor optical properties at room temperature due to their extremely strong electron–phonon coupling interaction. In this study, a doping strategy is employed by introducing Pb 2+ into Cs 2 InCl 5 ·H 2 O, resulting in the achievement of an efficient broadband blue emission, with a photoluminescence quantum yield (PLQY) of 58%. The temperature-dependent PL spectra reveal that the efficient emission is attributed to the weakening of the electron–phonon coupling strength in the lattice and the inhibition of the phonon-assisted non-radiative recombination process through Pb 2+ doping. The validity of this deduction is further corroborated by the results of the Raman spectra. The results of the first-principle calculation demonstrate that the broadband emission originates from multiple emission paths in In 3+ and Pb 2+ polyhedrons. In addition, Pb 2+ -doped Cs 2 InCl 5 ·H 2 O can realize the transformation from sky-blue emission to deep-blue emission by absorbing water in the air. Remarkably, this change is reversible during the heating–cooling cycles, demonstrating excellent optical stability with repeatable recyclability.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Wangjiang Gao,Chenglong Wang,Hexing Yang,Chunjing Ran,Shengzhou Xu,Dan Ren
Optimizing the electrocatalytic interface for the electroreduction of carbon dioxide (CO 2 ) in acid through the usage of cations in the electrolyte has shown its effectiveness in enhancing CO 2 conversion efficiency. However, such a positive impact in promoting CO 2 activation is limited by the solubility of salt, hence alternative ways to optimize the interface shall be sought for. Here, the hydrophobicity of the catalytic interface is tuned through the judicious design of a sandwich-like structure by covering the catalytic copper layer with polytetrafluoroethylene (PTFE) particles. After optimizing the thickness of the PTFE layer on a commercial CuO X nanoparticle catalyst, an improved FE for multi-carbon products from 35.0% to 59.3% in 0.05 m H 2 SO 4 electrolyte with the addition of 0.8 m K + (pH = 1.6) is achieved. Moreover, in situ Raman spectroscopy proves that the hydrophobic layer facilitates the formation of * CO intermediates and promotes the transition of bridge-bonded * CO to atop-bonded * CO. The reduction of carbon monoxide (CO) is further performed at different partial pressures to reveal the critical role of * CO coverage for the formation of multi-carbon products. Collectively, it is proposed that the optimized hydrophobic modification of the catalyst effectively tunes the coverage of * CO intermediate as well as reduces the available water molecules at the interface, thereby promoting the formation of multi-carbon products and simultaneously suppressing hydrogen evolution reaction. The study illustrates a new venue toward improving the efficiency of CO 2 conversion in acid.
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高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Zhou Jie,Li Jie,Kan Liang,Zhang Lei,Huang Qing,Yan Yong,Chen Yifa,Liu Jiang,Li Shun-Li,Lan Ya-Qian
Mimicking natural photosynthesis to convert CO 2 with H 2 O into value-added fuels achieving overall reaction is a promising way to reduce the atmospheric CO 2 level. Casting the catalyst of two or more catalytic sites with rapid electron transfer and interaction may be an effective strategy for coupling photocatalytic CO 2 reduction and H 2 O oxidation. Herein, based on the MOF ∪ COF collaboration, we have carefully designed and synthesized a crystalline hetero-metallic cluster catalyst denoted MCOF-Ti 6 Cu 3 with spatial separation and functional cooperation between oxidative and reductive clusters. It utilizes dynamic covalent bonds between clusters to promote photo-induced charge separation and transfer efficiency, to drive both the photocatalytic oxidative and reductive reactions. MCOF-Ti 6 Cu 3 exhibits fine activity in the conversion of CO 2 with water into HCOOH (169.8 μmol g −1 h −1 ). Remarkably, experiments and theoretical calculations reveal that photo-excited electrons are transferred from Ti to Cu, indicating that the Cu cluster is the catalytic reduction center.
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PubMed
高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
shuailong Song,Zhinan Wu,Tong Zhou,Yunxia Wen,Wei Cao,Han Lin,Xiaohua Lu,Tuo Ji,Jiahua Zhu
The major challenge that solid amine sorbents face in practical large-scale applications is their susceptibility to degradation under humid and oxygen-containing conditions. This study developed a superhydrophobic alkyl-silica by co-hydrolyzing alkyl-silane and tetraethyl orthosilicate and then immobilizing polyethyleneimine as a CO2 sorbent. By adjusting the chain length and density, the surface of the alkyl-silica has abundant alkyl chains, and the PEI molecules are intercalated into the surface alkyl layer. These alkyl chains effectively block the contact of O2 and H2O with the amine group, thereby selectively allowing the adsorption/desorption of CO2 molecules through the alkyl layer. The results showed that the working capacity of PEI/alkyl-silica was maintained at 86% by oxidation treatment and 85% by rinsing treatment, respectively, exhibiting excellent stability compared to unprotected PEI/SiO2. Meanwhile, the alkyl chain due to the steric hindrance effect weakens the interaction between CO2 and amine and does not reduce its original working capacity. The energy consumption of PEI/alkyl-silica during regeneration was lowered to 1.24 GJ·t-1-CO2. This interfacial building concept provides a new path for designing a long-term stable amine sorbent for cost-effective CO2 capture by avoiding the contact of O2 and H2O with the amine.
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高影响因子
ADVANCED MATERIALS
·
2023
·Vol. 35
·期 41
·2304712
·
IF 29.4
Wenda Bao,Yue Zhang,Lei Cao,Yilan Jiang,Hui Zhang,Nian Zhang,Ying Liu,Pu Yan,Xingzhi Wang,Yixiao Liu,Haoyuan Li,Yingbo Zhao,Jin Xie
Incorporating plasticizers is an effective way to facilitate conduction of ions in solid polymer electrolytes (SPEs). However, this conductivity enhancement often comes at the cost of reduced mechanical properties, which can make the electrolyte membrane more difficult to process and increase safety hazards. Here, a novel crosslinking strategy, wherein metal-alkoxy-terminated polymers can be crosslinked by precisely controlling the content of H 2 O as an initiator, is proposed. As a proof-of-concept, trimethylaluminum (TMA)-functionalized poly(ethylene oxide) (PEO) is used to demonstrate that ultrafine Al–O nanoclusters can serve as nodes to crosslink PEO chains with a wide range of molecular weights from 10 000 to 8 000 000 g mol −1 . The crosslinked polymer network can incorporate a high concentration of plasticizers, with a total weight percentage over 75%, while still maintaining excellent stretchability (4640%) and toughness (3.87 × 10 4 kJ m −3 ). The resulting electrolyte demonstrates high ionic conductivity (1.41 mS cm −1 ), low interfacial resistance toward Li metal (48.1 Ω cm 2 ), and a wide electrochemical window (>4.8 V vs Li + /Li) at 30 °C. Furthermore, the LiFePO 4 /Li battery shows stable cycle performance with a capacity retention of 98.6% (146.3 mAh g −1 ) over 1000 cycles at 1C (1C = 170 mAh g −1 ) at 30 °C.
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高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Xinyu Wang,Mingyang Hu,Yun Liu
This study investigates a one-step process for the simultaneous separation of cellulose, hemicellulose, and lignin from lignocellulosic biomass using γ-valerolactone (GVL)/H 2 O pretreatment, which also converts hemicellulose to furfural (FF). A response surface methodology (RSM) was applied to optimize the process parameters. Under optimal conditions (163 °C for 1.5 h), the maximum FF yield reached 85.36 %, and cellulose purity was 80.80 %. The extracted GVL-lignin was characterized as low-molecular-weight guaiacyl-syringyl (G-S) type nanospheres with significant antioxidant activity. The conversion of hemicellulose to FF was enhanced by the synergistic interaction of Lewis acid (MgCl 2 ) and Brønsted acid (H 2 SO 4 ), which promoted the isomerization of xylose and dehydration to FF. The high-purity cellulose yielded 18.87 g/L ethanol through separate hydrolysis and fermentation (SHF), 27 times higher than untreated solids. Additionally, GVL exhibited consistent performance in lignocellulose separation after six cycles. This method offers an efficient and sustainable approach to valorize lignocellulosic biomass, advancing the production of high-value products.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xiaoyan Zhang,Wenkang Ni,Peihang He,Zhijie Wang,Ke Wang,Zizhong Zhang,Wenxin Dai,Xianzhi Fu
Photocatalytic CO 2 reduction comprises two coupled half-reactions: CO 2 reduction and H 2 O oxidation. Efficient coupling of these reactions maximizes the utilization of photogenerated electrons and holes, enhancing CO 2 conversion and product selectivity. In this study, sulfur-deficient V S -Zn 3 In 2 S 6 (V S -ZIS) catalysts were synthesized via an ethylene glycol solvothermal method, followed by anchoring Fe single-atom sites (Fe/V S -ZIS) to facilitate CO 2 photoreduction using H 2 O as proton source. The 1 %Fe/V S -ZIS exhibited exceptional performance, with a CO production rate of 88.6 μmol·g −1 ·h −1 and 97 % selectivity. Experimental and DFT results revealed that V S functioned as reductive sites to strengthen CO 2 adsorption and activation, while Fe single atoms (SAs) served as oxidative sites to facilitate H 2 O dissociation for proton supply. Fe SAs also induced spin polarization to enhance IEF, thereby suppressing photogenerated charges recombination at redox sites. Meanwhile, Fe SAs reduced COOH* formation energy barrier and lowered CO desorption temperature, improving CO selectivity. The constructed dual active sites synergistically enhanced the overall photocatalytic CO 2 reduction performance. This work offers new technical pathways for designing redox dual-active sites to boost the overall photocatalytic CO 2 reduction efficiency.
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高影响因子
FUEL
·
2023
·
IF 7.4
Xin Huang,Zijun Ran,Zhi He,Jingyu Ran
Mercury has a significant impact on environment and is mainly derived from coal-fired power plant. Herein, we report a potential route for efficient removal of Hg 0 via oxidation reactions using Ce-doped LaCoO 3 supported on CeO 2 catalyst. Catalyst characterization results proved that Ce can successfully substitute a desired part of Co into the LaCoO 3 crystal lattice via a sol–gel method. The Hg 0 removal experiments suggest that Hg 0 removal efficiency decreased in the order of La 0.875 Ce 0.125 CoO 3 /CeO 2 > La 0.875 Ce 0.125 CoO 3 > LaCoO 3 . The presence of O 2 provided more active oxygen and resulted in approaching 100% Hg 0 removal efficiency. Introducing H 2 O and sole SO 2 would significantly reduce the Hg 0 removal efficiency as a result of competitive adsorption on the actives sites of the catalyst. On the other hand, SO 2 could reacted with Hg 0 in the presence of O 2 and thereby recover the high Hg 0 removal efficiency and the La 0.875 Ce 0.125 CoO 3 /CeO 2 catalyst presented a good performance towards sulfur resistance. Furthermore, the catalyst still exhibited a high Hg 0 removal efficiency performance after five times consecutive recycles.
研究领域:
环境科学
·
催化
·
材料科学
·
能源工程
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高影响因子
Journal of Saudi Chemical Society
·
2023
·
IF 5.6
Zhong-Lin Zang,Qi Wang,Zhi-Chao Dong,Sheng-Yao Huang,Hao-Zeng Wu,Cheng-He Zhou,Gui-Xin Cai
α,β -Unsaturated ketone is one of the important building blocks of the plenty of alkaloids, spices and pharmaceutical agents. Herein, we describe a peroxide-free electrochemical strategy to realize site-selective allylic C − H oxidation for the synthesis of α,β -unsaturated ketones. This electrochemically driven oxidation exhibits a broad substrate scope. Mechanistic investigations of this reaction uncovered HOAc and H 2 O as the oxygen source to achieve peroxide-free electrochemical allylic C − H oxidation.
研究领域:
有机化学
·
电化学
·
合成化学
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
En-Hui Yuan,Meng Li,Ming-Hui Yang,Xiaosheng Huang,Kun Zhang,Weiliang Han,Zhicheng Tang,Zhong-Wen Liu
A direct hydrothermal synthesis strategy is developed to prepare the Cu–Fe-ZSM-5 zeolites by using the ethylenediaminetetraacetic acid disodium dihydrate (EDTA-2Na·2H 2 O) chelated Cu 2+ and Fe 3+ precursors as metal sources. During the crystallization, the metal chelates were spontaneously embedded into the ZSM-5 crystals and subsequently transformed to the zeolites encapsulated copper and iron species after removing the chelating agent via the high-temperature calcination . Rigorous characterizations indicate that the resulted Cu 2+ /Cu + and Fe 3+ /Fe 2+ species are formed ultra-small nano-composites with an average diameter of ∼2.2 nm and highly dispersed in the ZSM-5 zeolite crystals. The acidity of the ZSM-5 zeolites is subtly modulated by the encapsulated Cu–Fe nano-composite. As expected, the as-prepared Cu–Fe-ZSM-5 exhibits outstanding catalytic performance for the selective catalytic reduction of NO x with ammonia (NH 3 -SCR) in the broad reaction temperature ranges of 220–480 °C, which is much better than the Cu–Fe/ZSM-5 prepared with the conventional wetness impregnation method. Furthermore, the resultant zeolites show high stability and good tolerance to H 2 O and SO 2 , and it is very competitive for practical application to eliminate NO x . The developed one-pot hydrothermal synthesis route by using EDTA-2Na·2H 2 O as chelating agent is very convenient and easily reproducible, providing a general guideline to design and fabricate the superior transition metal modified zeolite catalysts for NH 3 -SCR and the related reactions.
研究领域:
催化
·
环境科学
·
材料科学
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DOI
高影响因子
Molecular Catalysis
·
2017
·
IF 0
Peng Sun,Rui-tang Guo,Shu-ming Liu,Shu-xian Wang,Wei-guo Pan,Ming-yuan Li,Shuai-wei Liu,Jian Liu,Xiao Sun
CeSmOx mixed oxide catalysts supported on TiO 2 prepared by coprecipitation method were used for selective catalytic reduction of NOx with NH 3 . The results showed that the addition of Sm could effectively enhance the low-temperature SCR activity and SO 2 /H 2 O resistance of Ce/TiO 2 catalyst, and the appropriate mole ratio of Sm to Ce was 0.3. Characterization results indicated that the introduction of Sm could promote the formation of Ce 3+ and chemisorbed oxygen species on catalyst surface, which was favorable to the generation of NO 2 . Moreover, the doping of Sm could also promote the adsorption of NH 3 and NOx species on Ce/TiO 2 catalyst. The results of in situ DRIFT study revealed that the NH 3 -SCR reaction over CeSm/TiO 2 -0.3 catalyst was mainly controlled by the Langmuir−Hinshelwood mechanism in the low temperature range (<200 °C). Thereafter, the promoted NO oxidation and the enhanced NH 3 adsorption should play a major role for the excellent low-temperature SCR performance of CeSm/TiO 2 -0.3 catalyst.
研究领域:
催化
·
环境科学
·
材料科学
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