Surfaces and Interfaces
·
2024
·
IF 5.7
Binbin Wu,Chaorui Xue,Chi Zhang,Jinfang Zhang,Qing Chang,Caihong Hao,Lei Liu,Ning Li,Xiangqian Fan,Shengliang Hu
At present, the limited efficiency in ammonia generation poses significant challenge to the widespread practical implementation of photocatalytic nitrogen reduction to ammonia (PNRN). In this study, we synthesized a nanoporous TiO x powder (Alloy-RTO) by rapid breakdown anodization of TA13 alloy and subsequent magnesiothermic reduction. The Alloy-RTO exhibited superior photothermal and photocatalytic properties owing to its multicomponent and interconnective nanoporous structure, and the electronic band structure is suitable for efficient PNRN. Notably, through synergistic integration of PNRN with solar-driven interfacial water evaporation technology (SDIWE), the ammonia production rate was further enhanced, and a multifaceted role of SDIWE in enhancing PNRN was proposed: (1) increasing temperature of Alloy-RTO to promote PNRN; (2) raising temperature to accelerate ammonia water decomposition and facilitate PNRN; and (3) generating plenty of gaseous water to accelerate PNRN. This study presents an effective strategy for preparing nanoporous TiO x and highlights the pivotal role of SDIWE in promoting PNRN.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Hongchun Sun,Cui Dong,Chao Feng,Hui Wang,Zhenping Qu
Co 3 O 4 catalysts possess high activity in selective catalytic oxidation of NH 3 (NH 3 -SCO), but the low N 2 selectivity hinders their potential application. To enhance N 2 selectivity, the chemical bonded Nb-O-Co catalyst by the deposition of Nb species onto Co 3 O 4 (Nb/Co 3 O 4 -0.03) is constructed. It shows 100 % NH 3 conversion and 82 % N 2 selectivity at 180°C, and the N 2 selectivity is 2.2-fold higher than that of Co 3 O 4 (38 %). The failure of enhancement in N 2 selectivity for physically mixed Co 3 O 4 and NbO x (NbO x |Co 3 O 4 -0.03) further indicates the crucial role of chemical bonded Nb-O-Co in enhancing N 2 selectivity. In situ diffuse reflectance infrared Fourier transform spectra and NH 3 temperature-programmed desorption results show the formation of new NH 3 adsorption sites. Importantly, intermediates NO - stabled on Nb/Co 3 O 4 -0.03 tends to react with -NH 2 to produce N 2 through internal selective catalytic reduction (iSCR). This work offers insights into enhancing the N 2 selectivity in NH 3 -SCO and advances understanding of iSCR mechanism.
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高影响因子
FUEL
·
2024
·
IF 6.7
Xin-Yue Wang,Yi-Ming Gu,Xu-Peng Zong,Sheng-Sheng Zhao,Shu-Dong Wang
The inevitable combustion of fossil fuels in human industrial activities results in significant greenhouse gas emissions, leading to the pressing challenge of CO 2 /N 2 separation in humid flue gas. Iron-based Metal-organic frameworks (MOFs) have proven to be cheap, robust against water vapor attack due to the enhanced coordination bonds. In this study, we present two distinct MOFs i.e., DNL-9(Fe) and PCN-233(FeM II ), constructed by Fe clusters and 2,5-furandicarboxylic acid ligands. Static adsorption experiments revealed that DNL-9(Fe), featuring an exclusive Fe-F-Fe spiral packing structure, exhibited higher surface areas and enhanced CO 2 adsorption performance that outcompeted PCN-233 candidates. DNL-9(Fe) demonstrated a high IAST selectivity of CO 2 /N 2 at 247 (15/85, v/v, P/P 0 = 0.01), superior to the most of state-of-the-art Fe-MOFs reported up to date. The further theoretical calculations elucidated the binding sites of the framework with CO 2 molecules. Importantly, DNL-9(Fe) showed sufficient water stability and cyclic separation, as confirmed by dynamic breakthrough tests, indicating it as a promising candidate for practical CO 2 capture from humid flue gas.
研究领域:
化学
·
材料科学
·
环境科学
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高影响因子
FUEL
·
2022
·
IF 8.035
Xiaojun Dai,Yan Cheng,Meng Si,Qiang Wei,Dongdong Chen,Wenbin Huang,Yasong Zhou
A series of SAPO-11 molecular sieves were synthesized in the concentrated gel system by reducing the water content in the synthesis system. With SAPO-11 molecular sieves as supports, NiW-supported catalysts were prepared for the hydroisomerization of n-hexadecane. SAPO-11 molecular sieves and catalysts were characterized by XRD, SEM, N 2 adsorption–desorption, NH 3 -TPD, Py-IR, HRTEM and XPS. The results showed that reducing the water content in the synthesis system could increase the mesoporous volume of SAPO-11 molecular sieve and improve the acidity of SAPO-11. For the corresponding catalysts, using SAPO-11 synthesized in concentrated gel system as the support weakened the interaction between the active phase and the support, and increased the dispersion and stacking number of the active phase, which effectively improved the catalytic performance of the catalyst. The yield of i-hexadecane of the catalyst NiW/45W-SA corresponding to SAPO-11 synthesized in conventional water content system was 28.14%, while that of the catalyst NiW/5W-SA corresponding to SAPO-11 synthesized in concentrated gel system was 52.24%. According to the distribution of isomers, it is inferred that hydroisomerization of n-hexadecane over NiW/SAPO-11 follows the pore-mouth mechanism.
研究领域:
催化
·
材料科学
·
化学工程
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DOI
高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Qiang Xian,Xin Xiao,Jiaping Yu,Yi Gan,Li Chen,Xinmiao He,Enchao Wang,Hui Dan,Lin Zhu,Yi Ding,Tao Duan
The immobilization of iodine waste suffers from serious iodine loss during heat treatment. Herein, we reported on the high iodine retention immobilization of simulated radioiodine-contaminated Bi0–SiO2 sorbent in B–Bi–Zn oxide glass using Bi2O3 as a stabilizer under a N2 atmosphere. The effects of the Bi2O3 content and sintering atmosphere on the iodine immobilization behaviors (iodine retention ratio, phase composition, microstructure, and chemical stability) were investigated. It was found that the decomposition of BiI3 was prevented by adding Bi2O3 and sintering in a N2 atmosphere. The iodine retention ratio in the obtained glass waste form was significantly enhanced with increasing Bi2O3 content and sintering in the N2 atmosphere due to the synergistic effect. The achieved record-high iodine retention (92.22 ± 2.6%) was much higher than that of conventional heat treatment route (18.01 ± 3.5%). The results demonstrated that iodine was effectively immobilized through the formation of stable BixOyI (Bi5O7I and BiOI). Furthermore, the obtained iodine waste form exhibited excellent compactness and chemical stability. Owing to its high iodine retention ratio, this route can be employed to effectively immobilize radioactive iodine.
研究领域:
材料科学
·
核废料管理
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DOI
高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 36
·20945-20951
·
IF 10.733
Xue Zhao,Chen Yao,Hao Chen,Yunfan Fu,Changjun Xiang,Suhang He,Xiaohai Zhou,Haibo Zhang
Ammonia has been obtained from the Haber–Bosch process for decades, which requires an unendurably high temperature and high pressure. Alternatively, electrochemical conversion of N2 to NH3 turns out to be a promising method with much lower energy consumption and accessible reaction conditions. In this work, a novel nano-gold catalyst supported on a boron organic polymer (Au/M-BOP) was prepared and achieved both excellent ammonia yield and faradaic efficiency at low potential (r(NH3): 45.54 μg h−1 cm−2 or 75.89 μg h−1 mgcat.−1 FE: 10.35%), results that are close to the top of the pyramid compared to published literature results. Moreover, the catalyst is conveniently accessible through a pre-immobilized in situ reduction, and can maintain its electrocatalytic activity for multiple uses, which could have potential implications in the industrialization of the electrocatalytic production of ammonia.
研究领域:
材料科学
·
电化学
·
催化化学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Runlin Han,Faxiang Feng,Zanming Zhu,Guilin Dong,Xiaobing Liu,Minggang Guo,Xiaohang Yang,Jiahao Qin,Huahao Wang,Yan Dai,Gaohong He
Metal-organic frameworks (MOFs) based Mixed-matrix membranes (MMMs) still present challenges in overcoming the traditional trade-off between permeability and selectivity in gas separation. Functionality of MOFs demonstrates great potentials in overcoming this issue. In this study, hierarchically structured multifunctional C@Fe 2 O 3 @ZIF-8 was proposed to construct strong adsorbed and low-resistance transport pathways enabling high CO 2 sieving through a “selective thermal etching” strategy. Leveraging the thermal stability difference between MIL-88 A(Fe) and ZIF-8, the core undergoes selective pyrolysis while preserving the crystalline ZIF-8 shell. The ZIF-8 shell enhances CO 2 /N 2 separation while optimizing interfacial compatibility, whereas the porous carbon core provides mesoporous structures for enhanced gas transport and ultramicroporous regions for improved CO 2 adsorption. Meanwhile, paramagnetic Fe 2 O 3 in the core layer enables optimized distribution of C@Fe 2 O 3 @ZIF-8 within the Pebax matrix. The C@Fe 2 O 3 @ZIF-8/Pebax MMM exhibits 216.46 % and 65.12 % improvements in CO 2 permeability and CO 2 /N 2 selectivity, respectively, over the Pebax matrix, exceeding the 2019 McKeown upper bound. This study pioneers a novel approach for constructing advanced multicomponent materials with customizable hierarchical structures by synergistically integrating high-throughput carbon channeling with MOFs molecular sieving technology.
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Shaohui Xiong,Xingyi Ou,Qingquan Liu,Yiwen Li,Juntao Tang,Guipeng Yu,Chunyue Pan,Shibo Guo,Sitong Li,Menghan Yong
Polymers of intrinsic microporosity (PIM) have attracted considerable attention in the development of mixed matrix membranes (MMMs) for CO 2 separation. A prominent challenge lies in engineering the spacing of the polymer matrix chains while eliminating non-selective interfacial defects. In this study, a CO 2 -philic triazine-based porous polymer, featuring robust hydrogen bond donating groups, was employed to fabricate a series of interfacial defect-free PIM-1 based MMMs (denoted as PIM-1/CSU-1). The interfacial adhesion and compatibility have been greatly improved due to the strengthened hydrogen bond interaction, which was systematically validated through variable-temperature infrared spectroscopy. Additionally, the formation of hydrogen bonds allowed for the regulation of the polymer matrix chain spacing, making the chain distance loose. Remarkably, the resulting membrane exhibited a CO 2 permeability of 13,429 Barrer and CO 2 /N 2 selectivity of 33.1—246.6% and 70.2% higher than pristine PIM-1, respectively, surpassing the latest Jansen/McKeown upper bound established in 2019, but also significantly exceed the performance of previously reported MMMs for CO 2 separation. The strategy of mitigating interfacial defects through the formation of hydrogen bonds between fillers and the polymer matrix emerges as a viable and effective method for fabricating gas separation membranes with exceptional separation capabilities.
研究领域:
材料科学
·
高分子化学
·
气体分离
·
膜技术
·
物理化学
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高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2026
·Vol. 71
·期 8
·3669-3680
·
IF 2.4
Wu Shasha,Li Wenyu,Yang Li,Chen Zhen,Qin Yuanhang,Yuan Lunyong,Sun Wei
This study systematically investigates the influence
of lithium
nitrate (LiNO 3 ) modification on the gas adsorption characteristics
of UiO-66. The adsorption isotherms for carbon dioxide (CO 2 ), methane (CH 4 ), and nitrogen (N 2 ) were acquired
within a pressure range of 0 to 20 bar. The results from the cyclic
testing indicate that the UiO-66–0.05LiNO 3 variant
exhibits commendable stability. Notably, the incorporation of LiNO 3 enhances the CO 2 adsorption capacity by 29.48%,
reaching 2.24 mmol·g –1 at a pressure of 1 bar.
This is attributed to the introduction of lithium ions, which enhance
the electrostatic interaction between CO 2 and the MOF.
Analysis of the high-pressure data reveals that the Langmuir–Freundlich
model provides the most robust fit, whereas the Langmuir and Dual-site
Langmuir models demonstrate increased discrepancies as pressure escalates.
According to calculations based on the Ideal Adsorption Solution Theory
(IAST), the maximum selectivity of the material for the CO 2 /CH 4 and CO 2 /N 2 mixtures is 11.5
and 56.0, respectively. These results suggest that LiNO 3 modification significantly enhances both the adsorption capacity
and the selectivity for CO 2 separation.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Yani Dong,Li Chen,Jiaxin Liu,Guangmin Ren,Tuo Guo,Qingjie Guo
Photocatalytic nitrogen reduction reaction (PNRR) is an important tool for advancing carbon neutrality. However, effective N 2 adsorption and activation, and the subsequent dissociation of water, remain major challenges in the PNRR. In this work, FeVO 4 -based catalysts co-modified with Pt nanoclusters (NCs) and single atoms (SAs) (Pt/FeVO 4 ) are synthesized and applied in the PNRR. The synthesized Pt/FeVO 4 catalyst achieves a NH 3 production rate of 35.14 μmol·g −1 ·h −1 , 3.2 times higher than that of the original FeVO 4 , and the photocatalytic nitrogen fixation performance remains at a high level of 80% after four cycles. Density functional theory (DFT) calculations and various characterization experiments results show that the Pt NCs in the Pt/FeVO 4 catalysts can effectively promote the adsorption and dissociation of water, and the active hydrogen (*H) generated from the dissociation of water can migrate to the neighboring Pt SAs through the spillover effect. The local electron concentration around Fe is altered by the Pt SAs, which enables the activation and hydrogenation of N 2 , and thus enhances the efficiency of PNRR. This research emphasizes the essential effects of the dual active sites of NCs and SAs with hydrogen spillover in PNRR, which provides novel concepts for the design of highly efficient catalysts.
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高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122841
·
IF 7.5
Mian Zhu,Chao Lyu,Xieding Sun,Xiaochuan Yang,Jingxian Liu
To develop high-efficiency carbon dioxide (CO 2 ) adsorbents featuring low-pollution and low-energy-consumption preparation, gel bead precursors were first fabricated via gelation of nanocellulose, polyvinyl alcohol (PVA), and 2-methylimidazole. A nitrogen-doped precursor derived from hydrothermal recrystallization of melamine and dextrin was uniformly incorporated into the gel matrix to construct a nitrogen-enriched system. Subsequently, ZIF-8 was grown in situ within the composite beads through immersion in a zinc ion solution, yielding a biomass-polymer@ZIF-8 support after drying, which was then carbonized under N 2 to produce nitrogen-doped porous carbons. Based on static CO 2 adsorption evaluations across 15 sample sets at 0 ℃ and 25 ℃, 800 °C was identified as the optimal carbonization temperature. The sample CZN-II-800, with 4.31% external nitrogen doping in the precursor, exhibited absolute CO 2 adsorption capacities of 3.39 mmol/g at 0 ℃ and 3.08 mmol/g at 298 K (1 bar), which was 66.5% higher than that of its nitrogen-free counterpart CZ-800. Additionally, it displayed a CO 2 /N 2 selectivity coefficient of 8.9 under dynamic competitive adsorption conditions at 1 bar and 298 K. This work therefore establishes a scalable hybrid route integrating biomass materials with ZIFs to design high-performance adsorbents for efficient CO 2 capture from flue gases.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Shaozhi Liu,Honggang Zhang,Guangyao Zhai,Zeyan Wang,Hefeng Cheng,Peng Wang,Zhaoke Zheng,Ying Dai,Baibiao Huang,Yuanyuan Liu
Ozonation assisted photocatalytic (OPC) nitrogen oxidation provides a new sustainable strategy for nitrate production, yet the inefficient activation of N 2 and the rapid recombination of photogenerated carrier remains a challenge. Herein, the BiOBr-based catalysts with Mn single atoms and oxygen vacancies is designed for the OPC N 2 oxidation. Under optimal conditions, the yield of NO 3 − over Mn 0.035 /O v -BiOBr is as high as 151.3 μmol g −1 h −1 , which are 7.63 times that over BiOBr (19.8 μmol g −1 h −1 ). Detailed experimental analysis reveals a synergistic effect between Mn single atoms and oxygen vacancies, where Mn single atoms act the active site for N 2 adsorption and reaction, and oxygen vacancies for O 3 activation and transformation. Theoretical calculations further demonstrate that the synergistic effect between Mn single atoms and oxygen vacancies not only enhance the dipole moment along the [001] direction (i.e. the interlayers), but also induce a dipole moment within the [Bi 2 O 2 ] 2+ layer, both of which are advantageous for chare separation and the subsequent transformation of O 3 to reactive oxygen species (ROS). Meanwhile, a variety of active species act cooperatively to sped up the N 2 oxidation process. This work provides a new method for efficient N 2 oxidation to NO 3 − , namely photocatalytic ozonation, and also provides a deep understanding for the modulation of the internal electric field (IEF) effect of BiOBr via both single atoms and oxygen vacancies to improve charge separation.
研究领域:
催化
·
环境科学
·
材料化学
·
光催化
·
可持续化学
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高影响因子
危险品化学品经营许可证（带存储）