APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Huiyuan Cheng,Jingwei Hu,Zihan Liu,Guangping Lei,Guojun Xi,Yayun Zhang,Hantao Liu,Xuhuan Guo,Huiyun Ren
Developing novel adsorbents for CO 2 capture and separation offers an efficient approach to relieving global environmental problems. To promote CO 2 capture from flue gas, novel Cr 3 O@MIL-101(Cr) composites was synthesized through packing [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 into MIL-101(Cr) cages. The resultant composite Cr 3 O@MIL-101(Cr) presents higher CO 2 uptakes at lower pressure ranges, benefiting from the increased content of unsaturated Cr(III) ions and micropores relative to MIL-101(Cr). Meanwhile, IAST selectivity for CO 2 /N 2 mixture reached 50.2 under standard temperature and pressure, outperforming most of the reported materials. Further GCMC simulations reveal that the synergistic effect of [Cr 3 O(HCOO) 6 (H 2 O) 3 ] + , NO 3 − and MIL-101 (Cr) could effectively facilitate the interactions with CO 2 molecules and hinder N 2 molecules from approaching the optimal adsorption sites. Thus the [Cr 3 O(HCOO) 6 (H 2 O) 3 ]NO 3 encapsulated MIL-101(Cr) can be recommended as a promising adsorbent for superior CO 2 /N 2 separation.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2024
·
IF 2
Yang-Dian-Dian Wang,Shi-Hua Sang,Han-Zhong Zhang,Ling-Xuan Wang
The solid–liquid phase equilibria of the ternary system LiBr–Li2SO4–H2O at 273.15, 288.15, and 308.15 K were investigated by the isothermal dissolution equilibrium method. The equilibrium solid phases were identified by X-ray powder crystal diffraction. The isothermal phase diagrams of the ternary system at different temperatures were drawn in detail. The equilibrium phase diagrams of the ternary system at 273.15, 288.15, and 308.15 K have one invariant point, two univariate curves, and two crystallization fields (corresponding to LiBr·2H2O and Li2SO4·H2O), respectively. The results show that LiBr has a strong salting-out effect on Li2SO4, and the solubilities of LiBr will be greatly improved with an increase in temperature. Furthermore, multiple linear regression and programming analysis are used to fit the single salt parameters (β(0), β(1), and Cφ) and the mixed ion interaction parameters (ψLi+,Br–,SO42–) of lithium salt at 288.15 and 308.15 K. The Pitzer model and particle swarm optimization (PSO) were used to predict the solubilities in the ternary system at multitemperatures, and the phase diagrams of calculation and experiment are drawn accordingly. The experimental results and model predictions are in good agreement, indicating that fitted ion interaction parameters in this work of the Pitzer model have good applicability.
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CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Yanru Zhu,Zhijun Zhang,Jian Zhang,Shuangjiang Jiang,Zhe An,Hongyan Song,Xin Shu,Wei Xi,Lirong Zheng,Jing He
ABSTRACT Photosynthesis is a potential strategy to enable endergonic process that usually needs high-temperature in thermochemistry to supply the energy for inert-bond activation and/or strong endothermic reaction . The conversion of CO 2 into value-added C 2 -oxygenates is a promising process to realize artificial photosynthesis , but suffers from relatively lower efficiency due to complex multi-electron (≥ 10) transfer processes and sluggish kinetics of C–C coupling. This work proposes an all-new H 2 O-promoted strategy for efficient production of C 2 oxygenates from the concurrent activation and subsequent co-conversion of CO 2 with CH 4 under photo-thermal cooperation, in which photocatalytic H 2 O-splitting derived active hydrogen species for CO 2 activation, and concomitant active oxygen species for CH 4 activation. A formation rate of as high as 2.05 mmol g −1 h −1 for C 2 -oxygenates (CH 3 CHO and CH 3 CH 2 OH) in a selectivity of > 86% has been afforded over SrTiO x supported CuCo under 200 °C and ultraviolet-visible illumination. It has been revealed that SrTiO x drives photocatalytic H 2 O-splitting under the excitation primary from ultraviolet light, paired Cu I /Cu 0 sites promote the formation of *CH x O intermediate from CO 2 , Co sites conduct CH 4 -to-*CH 3 , and C–C coupling of *CH x O and *CH 3 on adjacent Cu-Co facilitates the generation of C 2 -oxygenates.
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ACS Omega
·
2024
·
IF 3.7
Qingjing Liu,Ruisheng Wang,Ranjia Li,Xiaosheng Wang,Suoqi Zhao,Changchun Yu
Mn–Na2WO4-based catalysts with different supports were prepared using the incipient wetness impregnation method and evaluated for their oxidative coupling of methane (OCM) reaction performance. The results demonstrated that the SiO2- supported catalyst exhibited the best catalytic performance, and the introduction of H2O further enhanced its activity. Under the conditions of a feed gas mixture of CH4/O2/H2O = 6:1:24 at 800 °C and atmospheric pressure, the CH4 conversion and C2+ selectivity over the Mn–Na2WO4/SiO2 catalyst increased from 28.4% and 77.4% (without H2O) to 33.2% and 84.9%, respectively. In contrast, the catalytic activity using TiO2 and MgO supports drastically declined. Characterizations using X-ray diffraction (XRD), in situ infrared spectroscopy (In-situ IR), X-ray photoelectron spectroscopy (XPS), hydrogen temperature-programmed reduction (H2-TPR), and oxygen temperature-programmed desorption (O2-TPD) revealed that the introduction of steam not only served as a diluent to decrease the partial pressures of the reactants CH4 and O2, thereby reducing deep oxidation reactions in the gas phase, but also interacted with surface oxygen species (O22–) and silica to form adjacent surface-bonded disilanol free radicals Si–OIH. This interaction facilitated the dehydrogenation and coupling of two methane molecules on the catalyst surface, resulting in the generation of C2+ products, significantly enhancing the catalytic activity and selectivity of OCM.
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Small Structures
·
2025
·
IF 11.3
Jiaojiao Fan,Jianmin Chen,Wenji Li,Zhongxing Zhao,Zhenxia Zhao
Converting CO 2 into high-value-added products via “artificial photosynthesis” under mild conditions is a promising yet challenging strategy for developing efficient photocatalysts. This study reports a simple two-step solvothermal approach to fabricate the dual-metal–organic framework (MOF) nanocomposite NH 2 -UiO-66@PCN-224 (NU-66@PCN-224) with tightly integrated interfaces, which achieves efficient CO 2 to CO photocatalytic reduction under light irradiation. The epitaxially grown PCN-224, composed of Zr 6 clusters and tetrakis (4-carboxyphenyl) porphyrin (TCPP), serves as a shell layer and a visible light-absorbing antenna, thereby broadening the light absorption range of the composite material. Moreover, the tightly integrated interfaces of NU-66@PCN-224 enhance the mobility of photogenerated charge carriers, consequently enhancing its capability for CO 2 catalytic reduction. As a result, the combination of NU-66 and PCN-224 retains their individual advantages while achieving a synergistic enhancement of both adsorption and catalysis, further improving the photocatalytic performance. The as-prepared NU-66@PCN-224 catalyst exhibits outstanding photocatalytic performance, yielding 74.6 μmol g −1 h −1 of CO under irradiation without sacrificial agents or photosensitizers. This work demonstrates a straightforward and effective method for designing MOF-on-MOF photocatalysts with enhanced photoactivity.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Yushan Chen,Zhiwen Cheng,Hongbo Zhang,Jianxing Liang,Jingdong Li,Chenyu Bao,Shuxun Chen,Xi Wu,Zhujun Liu,Jinping Jia,Maohong Fan,Kan Li
The adsorption strength of H 2 O on the catalyst surface is a key factor in electrocatalytic hydrogen/oxygen evolution reactions (HER/OER). Excessive adsorption increases the energy barrier for intermediate formation, hindering HER/OER activity and stability. Here, a strategy is proposed for modulating lattice strain in 2D materials via 3D substrates. NiOOH/NiCu, a electrocatalyst with 2D film loaded on 3D branches, is synthesized on copper oxide nanowire arrays, and NiOOH compression strain is tuned within 0%–8.6% by controlling array diameter. In situ characterization and density functional theory calculations show that compressing NiOOH interlayer spacing weakens the adsorption of H 2 O and intermediates (*H/*O), lowers the Tafel step energy barrier and Gibbs free energy of *OOH formation, thus improving HER/OER activity. The 5.9% strained NiOOH/NiCu achieves HER and OER overpotentials of 18 and 197 mV at 10 mA cm −2 with Tafel slopes of 30.6 and 35.6 mV dec −1 , respectively, and operates stably at 1 A cm −2 for 1200 h in an alkaline anion-exchange-membrane electrolyzer.
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Energy Storage Materials
·
2025
·
IF 20.2
Xingyu Hu,Hui Shi,Yilei Zheng,Penghui Shao,Liming Yang,Xubiao Luo
The sustainable recovery of valuable metals from end-of-life lithium-ion batteries (LIBs) has become essential for relieving the supply-demand contradiction of key resources. However, the high similarity in physicochemical properties of transition metals poses a fundamental challenge for the selective recycling. Here we proposed a facile strategy for defining the demarcation line of precipitation/dissolution behavior for precise Ni/Co separation. A malonic acid-based deep eutectic solvent (DES) is developed, emphasizing the H 2 O-mediated competitive coordination and differentiated solubility. We discovered the distinctive formation of [Ni(H 2 O) 6 ] 2+ and [CoCl 4 ] 2- in the DES-20 % H 2 O system. Furthermore, the K sp differences of the Ni-complex and Co-complex in the C 3 H 2 O 4 2- -rich environment was effectively magnified. These significant differences synergistically enable the generation of C 3 H 2 NiO 4 ·2H 2 O precipitation (∼ 99.9 % purity), achieving a remarkable Ni/Co separation factor of 125, which guarantees sequential separation of all metals. This universal methodology along with in-depth mechanism understanding provides a guideline toward value-added recovery of LIBs.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Teng Zong,Ming Tian,Chaojie Wang,Nanxin Wang,Jiachen Yang,Lin Li,Yujia Han,Xiaodong Wang
It is of great significance but challenge to achieve superior H 2 O splitting performance by tailoring active sites in novel Fe-based mixed oxides in order to boost H 2 O activation to achieve the oxidation of metallic Fe to Fe 3+ back into parent substrate rather than thermodynamically more favourable Fe 2+ (Fe-O v ) usually exhibiting low H 2 O activation in chemical looping water splitting (CLWS). Herein, we for the first time reported the performance of Ga-doped garnets (Y 3 Fe 2 Ga x Al 3-x O 12 abbreviated as YF 2 G x Al 3-x , x = 1 and 2) for CLWS which surpassed most of the state-of-the-art Fe-based oxides by virtue of marvelous peak H 2 production rate of 195.3 mL min −1 g −1 , H 2 productivity of 60.7 mL g −1 , 100 % H 2 purity and outstanding redox stability for YF 2 G 2 A 1 . It was clarified that Ga doping led to the formation of an interface with Fe 0 and Ga δ+ -O v in garnets, which synergistically improved H 2 O dissociation, leading to the direct oxidation of Fe 0 to Fe 3+ back into garnets and thus accounting for its prominent performance.
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Soft Matter
·
2015
·Vol. 11
·期 35
·7059-7065
·
IF 4.029
Lei Hou,Peiyi Wu
The UCST-type transition of poly(acrylamide-co-acrylonitrile) (P(AAm-co-AN)) (molar fraction of AN: 13.3%; PDI = 3.2) in H2O and D2O is explored and compared by applying turbidity, DLS as well as FTIR measurements. The transition temperature of P(AAm-co-AN) in D2O is observed to be almost 10 °C higher than that in H2O at the same concentration, demonstrating a dramatic solvent isotope effect. Such a phenomenon could be rooted from a stronger interaction among polymer chains in D2O than in H2O, as indicated from DLS results. It is also observed in second-derivative analysis of FTIR spectra in the ν(CO) region, where all CO groups participate in the formation of inter-/intra-chain hydrogen bonds (CO⋯H–N) in D2O while there is still part of relatively “free” CO groups in H2O. Moreover, we find in the temperature-dependent FTIR spectra that CN groups exhibit hydrating behavior while CO groups present increased inter-/intra-molecular hydrogen bonding interaction (CO⋯H–N) upon cooling, revealing the later process to be the driving force of the UCST-type transition.
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CELLULOSE
·
2025
·
IF 4.8
Xin Weiming,Zhang He,Huang Weiwei,Zeng Rong,Gao Xia,Zhou Zuowan
Bamboo, as a renewable and biodegradable polymer resource, is currently used to develop environmentally-friendly polymer materials. However, obtaining bamboo-derived foam materials through sol–gel method encounters challenges in controlling pore structures and foam performance, primarily stemming from weak hydrogen bonding interactions among cellulose, hemicellulose and lignin. In this work, robust bamboo-derived foam materials are developed by freeze-drying all-component bamboo gels. To obtain gels with stable three-dimensional network structure, tannic acid (TA) is used to accelerate the sol–gel transition of the all-component bamboo suspension, by mediating the hydrogen bonding interactions among various biomass components. As a result, the gelation time is reduced from 60 h for the bamboo suspension down to 6 h for the TA/bamboo suspension. After freeze-drying the TA/bamboo gels, foam materials with a low density of ~ 0.08 g/cm 3 and satisfactory thermal insulation can be obtained. Notably the addition of TA not only preserves all components of the bamboo biomass in the foam materials, but also improves the compressive strength of the bamboo-derived foam material by 240% with respect to that pure bamboo foam. This study offers a sustainable and efficient approach for developing high-performance porous materials from all-biomass resources. Graphic abstract
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Advanced Optical Materials
·
2025
·
IF 7.2
Xiulan Shui,Shuangqiang Fang,BenLe Dou,Tianchun Lang,Haoliang Cheng,Jiaqi Ou,Zhou Zhou,Xuan Liu,Le Wang
Development of efficient sunlight conversion materials is critical for advancing sustainable agricultural practices, but current solutions often face challenges such as poor stability, high cost, and reliance on rare-earth elements. This study presents a rare-earth-free xCsMnCl 3 (H 2 O) 2 /(1−x)Cs 3 SbCl 6 heterojunction ( x = 1−0.65) synthesized via an eco-friendly mechanochemical method. By strategically combining Cs 3 SbCl 6 as a UV-absorbing donor with CsMnCl 3 (H 2 O) 2 as an efficient red emitter. The optimized heterojunction achieves a remarkable 36-fold enhancement at 626 nm (Full width at half maxima (FWHM) = 88 nm), perfectly matching chlorophyll a's absorption spectrum. Comprehensive experimental and theoretical analyses, including UV–vis absorption, photoluminescence (PL) spectroscopy, and density functional theory (DFT) calculations, reveal a dual enhancement mechanism: i) efficient interfacial electron-hole transfer and ii) suppression of non-radiative recombination through defect passivation. The practical application is demonstrated through a sunlight conversion film fabricated by embedding the 0.75CsMnCl 3 (H 2 O) 2 /0.25Cs 3 SbCl 6 composite in Ecoflex-0030, which exhibits exceptional environmental stability (90% PL retention after 90 days) and mechanical durability (500% tensile strain). The plant growth experiments confirm the film's agricultural efficacy, with chives and green cabbage growth rates increasing by 1.5- and 1.3-fold, respectively, compared to natural light conditions. This work not only addresses the limitations of existing light-conversion materials but also establishes a rare-earth-free, eco-friendly platform for energy-efficient agriculture.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Hong-Nan Chen,Yi-Fei Sun,Ming-Long Wang,Jin-Rong Zhong,Dan Rao,Chang-Yu Sun,Guang-Jin Chen
CO 2 hydrate provides an important alternative solution for CO 2 geological sequestration. However, fingering flow of liquid CO 2 and hydrate membrane effect can severely restrict flowing CO 2 conversion to hydrate. Here we report an enhanced CO 2 hydrate sequestration method via CO 2 -H 2 O emulsion injection, and its effectiveness has been proven in a three-dimensional system. Compared to liquid injection, emulsion injection demonstrated higher displacement efficiency of pore water and larger sweep area, finally increasing CO 2 sequestration density by 142 %. The highly dispersed CO 2 micro-droplets significantly increase CO 2 -H 2 O contact capability and weakens the hydrate membrane effect, thereby greatly increasing the rate and quantity of hydrate conversion. For different water contents, the highest CO 2 sequestration density of 148 kg/m 3 is achieved at 40 % water content, with hydrated CO 2 accounting for 71.45 %. The excellent performance of CO 2 -H 2 O emulsion provides a green and high-efficient approach to CO 2 hydrate sequestration.
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