CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jiejie Bai,Yue Shi,Aixin Ma,Feifei Liu,Yanru Liu,Caixia Li,Jianping Lai,Lei Wang
The production of three separated, high-value chemicals (H 2 O 2 , urea and H 2 ) from CO 2 , N 2 , and H 2 O represents a significant challenge. It is a prospective and innovative way to simultaneously produce these chemicals in an anion exchange membrane (AEM) electrolyzer, which couples anodic 2e - water oxidation (2e - WOR) and cathodic CO 2 , N 2 and water reduction reaction (CNWRR), but has not yet been realized. Here, we found that bifunctional Cu x Ti 1-x O 2-y catalysts can be employed in the electrochemical production of H 2 O 2 , urea and H 2 from CO 2 , N 2 and water, and the optimized Cu 0.12 Ti 0.88 O 2-y catalyst exhibits an excellent productivity of 11.8 μmol cm −2 min −1 , 0.3 mg cm -2 h −1 and 0.82 mmol cm -2 h −1 for H 2 O 2 , urea and H 2 at 4.0 V (50 mA cm −2 ) in AEM electrolyzer, respectively. Theoretical calculations reveal that the superior performance of the 2e - WOR and CNWRR is attributed to the Cu doping effect, which not only promotes the coupling of *OH but also optimizes the adsorption energy barriers of COOH* and NNH*. It is worth noting that the AEM electrolyzer assembled by bifunctional Cu 0.12 Ti 0.88 O 2-y reaches a current density of 50 mA cm −2 with a cell voltage of 4.0 V and exhibits excellent stability of 50-hour continuous operation.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Min Deng,Jing Wei,Zikang Qin,Zheng Yan,Junfeng Zheng,Lin Yang,Lu Yao,Wenju Jiang,Zhongde Dai
Styrene-butadiene-styrene triblock copolymer (SBS) has attracted increasing research attention due to its low cost, excellent mechanical properties, and superior gas permeability performance. In this work, a series of novel SBS doped membranes were prepared by introducing polyphosphoric acid (PPA), lithium 2,2,2- trifluoroacetate (TFALi), and 1,3-dichloro-1,1,3,3-tetraisopropyldisiloxane (Siloxane-Cl) into SBS as dopants. The results indicated that the addition of dopants into SBS membranes simultaneously enhanced the CO 2 permeability and CO 2 /N 2 selectivity of SBS membranes. Specially, doping Siloxane-Cl expanded the d-spacing, introduced flexible siloxane (Si-O) groups to enlarge molecular spaces, and formed more crosslinked network structure. Therefore, the SBS/Siloxane-20 membrane showed an approximately 4-fold increase CO 2 permeability compared to the pristine SBS membranes (from 203.3 to 842.9 barrer), accompanied by an increase in CO 2 /N 2 selectivity from 15.8 to 22.0. The obtained membranes also exhibited attractive anti-plasticization and anti-physical aging properties, no obvious decline in CO 2 permeability and/or CO 2 /N 2 selectivity can be observed after 1-week continuous permeation test, making them promising candidates for CO 2 /N 2 separation.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Bingqing Wang,Haofeng Sun,Jun Gao,Liying Kang,Haixiao Wan,Ying Wu,Hui Ma,Ziling Teng,Xian Xu,Lin Geng,Xiaozhi Wang,Li Ye,Yan Huang,Dongcui Li,Naisheng Jiang
Effective moisturizing agents are crucial for improving the performance of rinse-off cosmetic formulations. Herein, we explored the synergistic effects of trehalose and N 2 -(2,3-dihydroxypropyl)arginine hydrochloride (DPAH), a glycerol derivative of L-arginine, on enhancing surface deposition and moisturizing performance. Using various surface-sensitive characterization techniques, we observed significant enhancements in the surface deposition of the trehalose/DPAH mixture compared to trehalose alone or glycerol-based controls. Molecular dynamics simulations further revealed strong intermolecular hydrogen bonds between trehalose and DPAH, contributing to the observed synergistic effects. A moisture-retention study using a model anionic surfactant-based system demonstrated that the trehalose/DPAH mixture achieves higher skin hydration levels and reduced transepidermal water loss compared to trehalose and DPAH alone. These findings offer new insights into the molecular interactions that enhance the surface deposition and moisturizing efficacy of trehalose, presenting promising opportunities for developing advanced cosmetic formulations with optimized moisture-retaining properties.
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ACS Applied Polymer Materials
·
2025
·
IF 4.7
Mian Zhu,Chao Lyu,Bin Wang,Zhenhui Yu,Jingxian Liu
This study aimed to develop an effective CO2/N2 selective separation membrane for the capture of CO2 from air or flue gas. Polyvinylidene fluoride (PVDF) was chosen as the organic substrate for the preparation of mixed-matrix membranes (MMMs). To enhance the CO2 mass transfer rate, an ionic liquid (IL) with high CO2 solubility was introduced through direct material blending, while a leaf-like zeolitic imidazolate framework (ZIF-L) was functionalized with silane coupling agents as the inorganic filler. Subsequently, the prepared PVDF-IL@ZIF MMMs were tested for the CO2 separation performance and mechanical properties. The results revealed that IL loading could significantly enhance the separation performance of MMMs for CO2/N2 separation, and the AZL-incorporated IL loading MMM (PPAZL) exhibited the optimal gas separation performance, with 24.5% CO2/N2 selectivity at 2 bar transmembrane pressure. Notably, AZL also demonstrated superior interfacial compatibility with PVDF compared to both ZIF-8 and pristine ZIF-L, which facilitated the maximization of IL loading in the MMM, achieving more than 10% higher IL capacity than ZIF-8-filled counterparts while stabilizing IL immobilization within the membrane matrix.
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CERAMICS INTERNATIONAL
·
2022
·
IF 5.532
Luyan Yao,Changming Ke,Jinhua Zhang,Yuanbing Li,Bingqiang Han,Jingran Wang
Ti–Si–Fe alloys extracted from high-titanium blast furnace slag were utilized to replace part of the silicon powders, and then nitride/oxynitride bonded SiC ceramics were prepared by reactive sintering in graphite bed. Ti–Si–Fe alloys could react with CO/N 2 at a low temperature (1200 °C), and the addition of Ti–Si–Fe alloys could reduce the nitriding temperature of Si. Density functional theory calculations suggested that Ti–Si–Fe alloys enhanced reaction activity via weakening the strength of C O and N N bonds. The regional equilibrium phase diagrams of Si–C–N–O and Ti–Si–C–N–O under CO/N 2 atmosphere were calculated by thermodynamics. The change of whiskers morphology was observed by scanning electron microscope. Furthermore, the bulk density, the cold modulus of rupture, and the cold compressive strength improved with Ti–Si–Fe alloys content. The results showed that the addition of Ti–Si–Fe alloys not only significantly promoted nitriding of Si and formation of Si 3 N 4 whiskers, but also improved the mechanical properties of the samples.
研究领域:
材料科学
·
陶瓷工程
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Shuyu Wang,Shuang Cai,Xuefeng Liu,Yongmin Zhang,Yinjun Fang
How to recycle surfactant and retrieve hydrophobic organic contaminants (HOCs) in the remediation of HOCs-polluted soil by means of surfactant-enhanced soil washing (SESW) is still a significant challenge. Here, a proof-of-concept strategy for solubilizing a model HOC of phenanthrene (Phe) in artificial Phe-polluted sand and co-pricipitating surfactant-Phe from the SESW effluent by reversible tuning Krafft temperature (K T ) of surfactant via CO 2 /N 2 -bubbling was reported for the first time. In the presence of N,N,N’,N’ -tetramethyl-1,2-ethylenediamine (TEMDA), the K T of sodium alkyl sulphonates (C n AS, n = 12, 14 and 16) was reduced after CO 2 -bubbling because of the formation of TEMDA carbonates; in contrast, the TEMDA carbonates could be deprotonated after the removal of CO 2 by N 2 -bubbling, which enabled the K T to increase, allowing subsequent precipitation of C n AS. By alternating CO 2 - and N 2 -bubbling, the K T of C n AS-TEMDA could be reversibly switched over 10 cycles without causing obvious adverse distortions. The potential usage of this novel K T -tuning strategy was demonstrated in a conceptual C 12 AS-TEMDA-enhanced Phe-polluted sand washing. About 99.9% of Phe was solubilized by C 12 AS at room temperature, about 92% of C 12 AS and 99% of Phe could be co-precipitated, allowing both the total organic carbon and chemical oxygen demand of the residue wastewater were remarkably reduced to less than 25 mg L −1 after a simple and conventional treatment with active carbon and ion-exchange resin. The precipitated C 12 AS could be separated from Phe by a simple Soxhlet extraction.
研究领域:
环境科学
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化学工程
·
污染治理
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Qi Chen,Zefeng Yang,Yueling Chen,Jionghua Wu,Jimmy C. Yu,Ling Wu
The fabrication of single atoms on MIL-125(Ti) for photocatalytic ammonia synthesis. • SAs modulate the local electronic structure for charge mobility and separated active site. • The favorable N 2 activation and protons supply optimizes the reduction kinetics. • Magnetic field-induced spin flipping to charge utilization further boost the activity. Photocatalytic nitrogen fixation is an attractive alternative to the energy-intensive traditional ammonia synthesis. However, the major challenge is that most photocatalysts are limited by their low charge mobility, insufficient molecules activation and sluggish reaction kinetics. Herein, we integrated single atoms (Co, Fe, Ni) on MIL-125(Ti) functionalized with sulfhydryl (MIL-125(SH) 2 , MTS) to afford Co-MTS, Fe-MTS and Ni-MTS for photocatalytic nitrogen reduction. Through uniformly dispersed SAs (single atoms) coordinated with O and S atom, such intimate interaction and charge redistribution can efficiently regulate the unsaturated Ti sites for N 2 adsorption and activation. Moreover, the introduced SAs species also serve as separated active center for water oxidation to promote H 2 O adsorption and protons release, kinetically optimizing protons supply and energy barrier of rate rate-determining step for N 2 hydrogeneration. Benefited from the spatially separated metal node-SAs dual sites and favorable reaction energy barrier, the optimized Ni-MTS sample shows an ammonia yield rate of 72.6 μmol·g −1 ·h −1 with an apparent quantum efficiency of 0.49% at 400 nm. This can be further enhanced by magnetic field-induced spin flipping contributed to charge utilization. This work would inspire the development of other high-efficiency single atom/MOFs that combining molecular activation and protons supply for photocatalysis.
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ACS Applied Nano Materials
·
2026
·
IF 5.8
Sun Na,Wen Xue,Dai Kunlong,Ma Yanxi,Tian Shaohua,Xue Rui,Zhang Song
Combination of 131 I radioiodine therapy and photodynamic therapy represents a potential strategy for improving the treatment of differentiated thyroid cancer. Herein, we developed a silver single-atom carbon nitride photosensitizer (Ag 1 −N 2 ), which is activated by the in situ light source of 131 I Cherenkov radiation, for effective photodynamic therapy in differentiated thyroid cancer. Atomically dispersed Ag formed well-defined Ag−N 2 coordination sites on g-C 3 N 4 , which adjust the energy band structure, optimizes *OH desorption, and inhibits its excessive reduction, thereby promoting the one-electron reduction of H 2 O 2 into • OH and cascading reactive oxygen species amplification. Additionally, Ag 1 −N 2 showed preliminary tolerability. In combination with Na 131 I, Ag 1 −N 2 enhanced intracellular ROS generation, reduced TPC-1 cell viability by approximately 80%, and produced greater tumor-growth inhibition than either monotherapy. This study presents an in situ Cherenkov-activated silver single-atom nanoplatform that offers a promising combination-therapy strategy for differentiated thyroid cancer.
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2025
·
IF 3.8
Shuangjiang He,Junchang Wang,Chong Wang,Xiao Zhang,Sen Liang
The Mn-Fe-Co-Zn-O series is a widely used thermistor material, but its thermal stability is compromised by nitrogen glass encapsulation, limiting its application in electrical devices. To address this issue, La 2 O 3 and Y 2 O 3 were used as rare earth oxide dopants, and xR 2 O 3 -Mn 0.76 Fe 0.87 Co 1.07 Zn 0.3 O 4 (x = 0.0025, 0.005, 0.01, 0.02) negative temperature coefficient (NTC) materials were synthesized via solid-state sintering. The effect of rare earth doping on the electrical properties after high-temperature nitrogen annealing was investigated. After annealing at 750°C for 4 h, the variation in resistivity ( ρ 25 ) and material constant ( B 25/50 ) significantly decreases with increasing La doping. For the La-doped sample (x = 0.01), Δρ 25 decreased to 7.77% and ΔB 25/50 to 0.77% (for the Y-doped sample (x = 0.01), Δρ 25 decreased to 22.76% and ΔB 25/50 to 1.91%), compared to the undoped sample, where Δρ 25 reduced by 168.84% and ΔB 25/5 0 by 5.57%. This improvement was attributed to rare earth accumulation at grain boundaries, filling voids and forming R-O bonds, which inhibited oxygen vacancy migration and significantly reduced grain boundary resistance. Rare earth doping effectively improved the thermal stability and electrical consistency of NTC thermistor ceramics in high-temperature nitrogen atmospheres, offering a new strategy for high-temperature encapsulation applications. (Y-doped samples showed similar results, as detailed in the Supplementary Materials.)
研究领域:
材料科学
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无机非金属材料
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电子陶瓷
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热敏材料
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固态化学
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Huiyuan Cheng,Jingwei Hu,Shaoke Bu,Yushuang Shi,Guangping Lei
The escalating atmospheric concentration of CO 2 has intensified the demand for efficient carbon capture technologies. Here, an innovative composite adsorbent, Cu-Salophen@Cu-BTC, was successfully synthesized via an in-situ encapsulation strategy to enhance the selective adsorption of CO 2 from CO 2 /N 2 mixture. The incorporation of Cu-Salophen into the Cu-BTC framework was confirmed through XRD, ICP-OES, and FT-IR analyses. The composite exhibited a notable improvement in CO 2 uptake capacity, reaching 8.14 mmol g −1 (273 K) and 4.63 mmol g −1 (298 K) at 100 kPa, representing increases of 11.81% and 12.11%, respectively, compared to pristine Cu-BTC. Moreover, the CO 2 /N 2 separation performance was enhanced by 23.44% (273 K) and 36.06% (298 K). GCMC simulations revealed that the superior performance arises from the synergistic effects of additional adsorption affinities of CO 2 and real-time pore size regulation enabled by the mobile Cu-Salophen molecules. The composite also demonstrated excellent recyclability and improved water stability, underscoring its potential for industrial post-combustion CO 2 capture.
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JOURNAL OF POROUS MATERIALS
·
2023
·Vol. 30
·期 6
·2129-2137
·
IF 2.6
Tao Ruyu,Liu Hao,Xiang Pan,Lin Yichao,Zhou Junjie,Zhou Chen,Zhao Yayun,Tian Ziqi,Zhang Qiuju
Nanoscale Zr-based metal-organic framework (MIP-202) particles were successfully prepared via a seeds-assisted hydrothermal secondary synthesis. The uniformly-shaped MIP-202 particles exhibit excellent performance on selective CO 2 adsorption from CO 2 /CH 4 and CO 2 /N 2 mixtures. At 298 K and 1 bar, the uptake ratios of CO 2 /CH 4 and CO 2 /N 2 of MIP-202 particles are as high as 32.6 and 65.2, respectively. The IAST (ideal adsorbed solution theory)-predicted selectivities of CO 2 /N 2 (50/50, v/v) and CO 2 /CH 4 (50/50, v/v) reach to 4.5 × 10 10 and 102.2, respectively. The breakthrough experiments further demonstrate that the CO 2 /CH 4 and CO 2 /N 2 mixtures can be efficiently separated through an adsorption column packed with MIP-202 particles. In addition, the as-prepared MIP-202 particles had a low iso-enthalpy of adsorption of CO 2 of 32.95 kJ/mol, which is favorable for the regeneration of the adsorbent. Herein the as-prepared MIP-202 is a potential material for efficient separation of CO 2 from CH 4 or N 2 through an energy- and cost-saving CO 2 capture process.
研究领域:
材料科学
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环境化学
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能源工程
·
纳米技术
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ACS Catalysis
·
2023
·
IF 12.9
Yanfei Liu,Zhang Liu,Chengxiong Wang,Jie Xu,Jianping Ai,Xiao Liu,Aimin Zhang,Yunkun Zhao,Chun Du,Bin Shan
Supported Pt catalysts suffer from low reaction selectivity (<65% at 100% conversion) in the selective catalytic oxidation of ammonia (NH3-SCO) because of their intrinsic over-oxidation tendencies. Herein, a strategy based on facilitating byproduct NOx reduction to N2 is demonstrated at CuOx/PtCu catalysts, aiming to tackle the low selectivity challenge. This PtCu alloy sample with a CuOx-rich surface displays an N2 selectivity of 95%, while its turnover frequencies are the highest among reported supported Pt-based catalysts. The enhanced reaction activities and N2 selectivities are primarily attributed to the Pt-Cuδ+ dual-site synergies at the CuOx/PtCu interface, in which dual sites exhibit distinct NH3 adsorption, activation, and dehydrogenation behaviors. The Olat assisted internal selective catalytic reduction mechanism at CuOx/PtCu with N2O22– as the central intermediates is proposed. Density functional theory calculation and temperature-programmed surface reaction measurements show that the N–O bond in N2O22– tends to break simultaneously with the assistance of Ov in CuOx followed by the easy transition from N2O22– to N2, which serve as the origin of the high selectivity.
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