Nano Research
·
2020
·Vol. 13
·期 11
·2967-2972
·
IF 8.183
Wei Peipei,Geng Qin,Channa Ali Imran,Tong Xin,Luo Yongsong,Lu Siyu,Chen Guang,Gao Shuyan,Wang Zhiming,Sun Xuping
To develop highly efficient electrochemical catalysts for N 2 fixation is important to sustainable ambient NH 3 production through the N 2 reduction reaction (NRR). Herein, we demonstrate the development of vanadium phosphide nanoparticle on V foil as a high-efficiency and stable catalyst for ambient NH 3 production with excellent selectivity. The high Faradaic efficiency of 22% with a large NH 3 yield of 8.35 × 10 −11 mol·s −1 ·cm −2 was obtained at 0 V vs. the reversible hydrogen electrode in acid solution, superior to all previously studied V-based NRR catalysts. Density functional theory calculations are also utilized to have an insight into the catalytic mechanism.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
·
IF 5.107
Rui Ding,Wenji Zheng,Kai Yang,Yan Dai,Xuehua Ruan,Xiaoming Yan,Gaohong He
High permeability and selectivity are desirable for mixed matrix membranes (MMMs) based CO 2 separation. Herein, a microemulsion based mixed linker strategy is proposed to introduce amino groups during the growth of ZIF-8. Compared to post-synthetic modification, this method presents a less reduction in S BET of ZIF-8, which is beneficial for CO 2 adsorption. By controlling the ratio of 2-methylimidazole to 2-aminobenzimidazole, NH 2 -ZIF-8 with various morphologies and sizes were synthesized and serve as the filler to fabricate the MMMs for CO 2 capture. From the scanning electron microscopy (SEM), no obvious agglomerations or defects are observed in ZIF-8/Pebax MMMs, due to the amino groups in ZIF-8 can interact with the amide in Pebax chain, which can improve compatibility between ZIF-8 and Pebax. With the amino groups, NH 2 -ZIF-8 shows higher affinity with CO 2 than that of non-amine-functionalized ZIF-8, leading to an enhancement in the separation performances. When the MMM doped with 6 wt% of NH 2 -ZIF-8(10), the CO 2 permeability reaches up to 163.8 Barrer, which increases by around 53% and 107.6% in contrast with the ZIF-8/Pebax MMM and pure Pebax membrane. Besides, the CO 2 /N 2 selectivity is enhanced by around 10% and 27%, respectively. These results indicate that amine-functional modification by mixed ligands is a useful way to construct MOFs-based MMMs with high performance for CO 2 /N 2 separation.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yan-Mei Zhang,Wen-Wen Xie,Xiao-Xue Hu,Xin-Ru Chen,Heng Mao,Li-Hao Xu,Xin-Yu Shi,Tao Wang,Ying-Nan Feng,Zhi-Ping Zhao
Bioethanol has garnered widespread attention as a potential substitute for traditional fossil fuels. Focusing on the treatment of bioethanol fermentation exhaust is crucial for optimizing bioethanol recovery and achieving carbon dioxide (CO 2 ) purification. This study successfully achieved the large-scale synthesis of zeolitic imidazolate framework-8 (LSZIF-8), which was then incorporated into polydimethylsiloxane (PDMS) to fabricate large-area ZIF-8/PDMS/PVDF mixed matrix membranes (MMMs) for bioethanol recovery from fermentation exhaust via vapor permeation (VP) processes. The ZIF-8/PDMS/PVDF MMMs exhibited a 1.5-time increase in ethanol permeability and selectivity improved by 1.7 times compared to the PDMS/PVDF membrane. The mass transport behavior of ethanol and CO 2 molecules within the membrane, as well as examining the interactions between different components was systematically explored. It delves into the disparities in separation performance between PDMS/PVDF membrane and ZIF-8/PDMS/PVDF MMMs with nitrogen (N 2 ), water vapor as the third component. Notably, high-quality LSZIF-8 crystals serves as a crucial source of raw materials for the continuous preparation of high-performance MMMs, addressing the limitation of traditional nanoparticle fillers in terms of scalability for production. This study paving new avenues for purifying fermentation exhaust and recovering bioethanol, while simultaneously present significant potential for industrial applications.
✓ 已验证
产品关联
DOI
高影响因子
Advanced Healthcare Materials
·
2024
·
IF 10
Wenxiao Shi,Yu Feng,Jincheng Tang,Yichang Xu,Wang Wei,Lichen Zhang,Xinzhao Jiang,Zhouye Ding,Kun Xi,Liang Chen,Yong Gu
The innate immune response is crucial to the inflammation, but how neutrophils and macrophages act in bone repair and tissue engineering treatment strategies await clarification. In this study, we found N2 neutrophils release stronger “eat me” signals to induce macrophage phagocytosis which then polarize into the M2c anti-inflammatory phenotype. This is beneficial for bone repair. Guided by this biological mechanism, we filled a mesoporous bioactive glass scaffold (MBG) with HAMA hydrogel loaded with TGFβ1 adenovirus (Ad@H), constructing a genetically engineered composite scaffold (Ad@H/M). The scaffold not only has good hydrophilicity and biocompatibility, but also provides mechanical stress support for bone repair. Adenovirus infection quickly induces N2 neutrophils, upregulating NF-κB and MAPK signaling pathways through Toll-like receptor 4 (TLR4) to promote the inflammatory response and macrophage phagocytosis. Macrophages perform phagocytosis and polarize towards the M2 phenotype, mediating the inflammatory response by inhibiting the PI3K-AKT-NF-κB pathway, maintaining homeostasis of the osteogenic microenvironment. The role of Ad@H/M scaffold in regulating early inflammation and promoting long-term bone regeneration was further validated in vivo. In brief, this study focuses on the cascade of reactions between neutrophils and macrophage subtypes, and reports a composite scaffold that coordinates the innate immune response to promote bone repair. This article is protected by copyright. All rights reserved
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Ruxin Peng,Jihai Shao,Yuanlin Xie,Anwei Chen,Liang Peng,Qingru Zeng,Si Luo
Being that the influence of organic ligands on contaminant removal by nanoscale zero valent iron (nZVI) has been explored in quite a few studies, there is little information on reaction mechanisms of the ZVI-ligand system under different aeration conditions. The degradation of nitrobenzene (NB) by nZVI-oxalic acids (OA) was investigated under N 2 , O 2 and without aeration conditions. From the findings, it was evident that OA dramatically improved NB degradation by nZVI with all of the aeration conditions. Approximately 100% of NB was degraded by nZVI-OA+N 2 system after 60 min of reaction, followed in effectiveness by nZVI-OA+ without aeration (95%) as well as nZVI-OA+O 2 (85%). Operation parameters including OA concentration and pH had significant effect on the removal of NB in the nZVI-OA system. 3 mM OA concentration and pH 3.0 were found to be favourable. The Fe 2+ , total dissolved iron concentrations, pH and ORP values in the nZVI-OA systems had also been monitored. Intermediates and trapping experiments showed that reduction played a fundamental role in the NB degradation by nZVI-OA under N 2 or without aeration conditions. The formation of Fe(OA) 0 and Fe(OA) 2 2− complexes had lower standard ORP, which could improve the strength of reductant in the systems, and thus resulting in an increased degradation efficiency of NB by nZVI-OA+N 2 . Under O 2 aeration condition, the NB degradation process could be regarded as an oxidation . In the meantime, OA promoted the production of reactive oxidants species by speeding up the oxidation rates of Fe 2+ by O 2 and H 2 O 2 . Summarily, the improved reactivity of nZVI was largely as a result of the strong complexation ability of OA.
✓ 已验证
DOI
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 47
·29742-29751
·
IF 3.108
Maodong Xu,Wanqing Zhang,Xiaomei Pei,Jianzhong Jiang,Zhenggang Cui,Bernard P. Binks
Stable n-decane-in-water Pickering emulsions were prepared using positively charged alumina nanoparticles in combination with a trace amount of the anionic surfactant sodium dodecyl sulfate (SDS) as a stabilizer. Particles were hydrophobized in situ by adsorption of surfactant enhancing their surface activity. Emulsions can be readily demulsified by addition of an equal amount of a switchable surfactant, N′-dodecyl-N,N-dimethylacetamidine (DDAA), which can be transformed between a surface-active amidinium/cationic form and a surface-inactive amidine/neutral form by bubbling CO2 or N2, respectively. Following addition of cationic DDAA which prefers to form ion pairs with SDS, desorption of SDS from particle surfaces occurs and alumina particles are rendered hydrophilic resulting in demulsification of the emulsion. However, by bubbling N2 into the demulsified mixture, DDAA molecules are converted to the amidine/neutral form leading to collapse of the ion pairs and re-establishment of the in situ hydrophobization of particles. Stable Pickering emulsions can be prepared again following homogenization. This simple demulsification/re-stabilization cycle can be repeated several times. Experimental evidence including measurement of the adsorption isotherm, zeta potentials, extent of particle adsorption at droplet interfaces in emulsions and microscopy is given to support the postulated mechanisms.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Cleaner Production
·
2024
·
IF 9.7
Wanru Feng,Jingya Zhang,Jianguo Mi,Junsu Jin,Guolei Xiang,Hong Meng,Shisen Xu
The synthesis of structured CO 2 adsorbents with high separation selectivity, strong stability, and low cost to meet industrial needs is very challenging. Here, we synthesized an ultra-stable Zn-MOF (Zn 2 (3-amion-1,2,4-triazolate) 2 (oxalate), Zn 2 (Atz) 2 Ox), and adopted an efficient in-situ growth strategy to produce millimeter-sized spherical Zn 2 (Atz) 2 Ox@AFP (Amino-Functionalization Poly(acrylates), AFP) composite. Due to the heterogeneous crystallization induced by the nanoscale crystal seeds and the confined space of AFP, the three-dimensional (3D) Zn 2 (Atz) 2 Ox bulk crystals transformed into 2D nanosheets with higher CO 2 adsorption efficiency and faster kinetics. Zn 2 (Atz) 2 Ox@AFP has a high affinity for CO 2 (2.05 mmol g −1 at 0.05 bar and 313 K) while exhibiting an inhibitory effect for N 2 (only 0.051 mmol g −1 at 1.0 bar and 313 K), leading to an excellent ideal adsorbed solution theory (IAST) selectivity (2990 for CO 2 /N 2 (5/95, v/v)). Interestingly, Zn 2 (Atz) 2 Ox@AFP exhibits a unique gating effect on CH 4 adsorption, which further extends its application range to natural gas purification. Dynamic breakthrough experiments confirmed that Zn 2 (Atz) 2 Ox@AFP can selectively capture CO 2 in the simulated CO 2 /N 2 (5/95) and CO 2 /CH 4 (5/95) mixed gases.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Rong Yang,Jianan Liu,Xuemeng Sun,Cheng Wang,Baojiang Jiang
The application of photocatalysis for the production of high-purity and high-energy-density green ammonia holds substantial promise. However, the restricted light absorption efficiency and high recombination rate of electron-hole pairs present significant obstacles to its practical deployment. In this study, we enhanced the photocatalytic efficiency of N 2 fixation by engineering a Mott-Schottky heterojunction and incorporating hollow microreactors. We synthesized Hollow-ZnO (H-ZnO) using ZIF-8 as a precursor and subsequently deposited Cu nanoparticles onto the H-ZnO to create the H-ZnO/Cu photocatalyst. The hollow structure not only bolstered the catalyst’s light scattering and absorption capabilities but also reduced the path length for photogenerated electron transitions, thereby improving the efficiency of electron transport and effectively inhibiting electron-hole pair recombination. Under Xe lamp irradiation, the H-ZnO/Cu-3 photocatalyst achieved a superior NH 4 + yield of 68.1 μmol g −1 h −1 without the addition of any sacrificial reagents, representing a 7.5-fold enhancement over pure ZnO. This research offers a novel strategy for designing metal oxide photocatalysts derived from MOFs and developing cost-effective photocatalytic systems.
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Daming Feng,Lixue Zhou,Chang Liu,Hui Li,Yusheng Zhang,Yali Yao,Tianyi Ma
Electrocatalytic nitrogen reduction reaction (NRR) for the synthesis of ammonia (NH 3 ) is one of the green and mild methods of artificial nitrogen fixation, promising as an alternative to replace the existing industrial process. Under the requirements of green chemistry and sustainable development, the design and development of highly active and stable electrocatalysts is very important for improved synthesis performance. Mimicking from the natural nitrogenase, Fe and Mo based catalysts have attracted much attention due to their superior catalytic performance for N 2 adsorption and activation. In this work, an interfacial engineering strategy has been used to prepare a Fe, Mo-bimetallic electrocatalyst for the electrosynthesis of NH 3 . In detail, the pre-pyrolyzed biochar-based Fe 2 O 3 composites were decorated with nano-flowered MoS 2 /MoO 2 hybrids by a solvothermal process (MoS 2 /MoO 2 @Fe 2 O 3 /BC). As confirmed by the extensive characterization, the further modification not only introduced functional counterparts into the electrocatalysts but also regulated the morphology of the nanostructure. The electrochemical tests showed that the highest NH 3 yield rate of MoS 2 /MoO 2 @Fe 2 O 3 /BC was 4.87 μg h − 1 cm −2 and highest FE was 16.5% in 0.1 M Na 2 SO 4 . The catalytic stability and durability were also presented in the longtime electrolysis and cycling experiments. The improved catalytic performance of decorated catalyst, as evidenced by the comparison with Fe 2 O 3 /BC, is attributed to the increased electrocatalytic active area, the moderated hydrophilicity, and the synergistic effect of Fe, Mo-bimetallic active sites. This study provides a new perspective for the design and development of low-cost transition metal complexes as electrocatalysts for nitrogen reduction reactions.
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2024
·
IF 4.8
Kunpeng Liu,Yixuan Yu,Qi Wang,Lingtong Kong,Tianjun Sun
A comprehensive investigation was conducted to explore the adsorption behaviors of CH 4 over N 2 on ultra-microporous Al/Zr-FDCA frameworks, which were synthesized specifically using the eco-friendly and bio-sourced 2,5-furandicarboxylic acid (FDCA). Characterization results revealed that both Al-FDCA and Zr-FDCA exhibited similar specific surface area and surface groups, leading to comparable methane uptake per-unit mass at atmospheric pressure. However, the presence of Zr nodes generated ultra-micropores around 0.43 nm in size, leading to a pronounced affinity for CH 4 . Zr-FDCA demonstrated a higher CH 4 /N 2 selectivity (8.90) calculated from the isotherms compared to Al-FDCA (3.86). Furthermore, breakthrough experiments indicated that under the same dynamic conditions, Zr-FDCA exhibited 1.5 times higher CH 4 uptake per unit volume and 2.5 times higher CH 4 /N 2 selectivity when compared to Al-FDCA. Initially, a four-step VPSA process was simulated to investigate the separation of CH 4 /N 2 mixture, in which the effects of feed-gas flow rate, adsorption time, adsorption pressure, and desorption pressure in VPSA cycle were extensively evaluated to enhance the purity and recovery of methane. Subsequently, a six-step process was employed for further optimization, achieving a purity of 95.9 % and a recovery of 99.1 %. The obtained results demonstrated the reliability of the established model and highlighted the significant potential of Zr-FDCA for CH 4 /N 2 separation.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Chuanming Zhang,Chunyang Shen,Zhenggang Huang,Hongxin Xu,Yaxiong Zeng,Baohong Guan
Ammonia nitrogen (NH 4 + -N), which exists in the dominant form of ammonium ion (NH 4 + ) under the pH of 6.5–8.5, is one of the regular indexes and the most important pollutants in drinking water. The selective conversion of NH 4 + -N into harmless substances is urgently needed and also a great challenge. Herein we propose a new NH 4 + -N conversion pathway based on a catalytic ozonation process with birnessite-type MnO 2 (δ-MnO 2 ) catalysts. The δ-MnO 2 exhibits a superior performance for NH 4 + -N (1.0 mg/L) removal in adsorption (8.26 %) and oxidation (44.6 %) as well as up to 95.2 % of N 2 selectivity, surpassing almost all the reported O 3 -based catalysts. Unlike the traditional radical oxidation, a singlet oxygen ( 1 O 2 )-dominated nonradical oxidation pathway is confirmed for the efficiently selective conversion of NH 4 + -N to N 2 through the successive dehydrogenation, leading to a 15.0-fold enhancement in NH 4 + -N oxidation rate compared with ozone oxidation. The Mn(III)/Mn(IV) redox sites and surface lattice oxygen in δ-MnO 2 act as the active sites promoting the decomposition of O 3 into •O 2 − and then 1 O 2 via electrons transfer. In application, δ-MnO 2 catalytic ozonation effectively removes NH 4 + -N in real drinking water and presents excellent stability. This work finds a nonradical reaction mechanism in catalytic ozonation for NH 4 + -N selective conversion to N 2 , and solidly solves the problem of low-concentration NH 4 + -N removal from drinking water under the limited pH of 6.5–8.5 condition.
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Hao Zhang,He Li,Mengyang Xia,Ben Chong,Honghui Ou,Yang Li,Xiaoqing Yan,Bo Lin,Guidong Yang
Urea synthesis via N2 and CO2 electrocatalysis has attracted significant interest but is hindered by unclear conversion mechanisms and low catalytic efficiency. Here, we report three atomically thin PdIn bimetallene catalysts, from surface-ordered Pd4 tetramers to linearly arranged Pd atoms, where the Pd–In dual-site atomic geometric configuration is tuned by introducing polyamine ligands to induce a steric hindrance effect. Experimental data and simulations show that the atomically thin structure enhances the exposure of internal sites, where Pd and In act as activation centers for N2 and CO2, respectively. Notably, on the orthorhombic Pd2In surface, an ordered Pd3 trimers nitrogen activation region exists, enabling the transformation of nitrogen from initial end-on to more favorable side-on adsorption in the C–N coupling intermediate. This transformation highly activates the N–N group in the *NCON intermediate, promoting proton hydrogenation. Consequently, Pd2In with ordered Pd3 trimers achieves a high urea yield of 5.69 ± 0.12 mmol g–1 h–1 and a Faradaic efficiency of 31.8 ± 0.3% at an ultralow potential of −0.1 V vs the reversible hydrogen electrode, marking one of the highest values in N2 and CO2 coreduction systems.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）