ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Yanwei Sun,Chunshan Song,Xinwen Guo,Yi Liu
Preferred orientation has proven to exert a significant impact on the gas separation performance of metal–organic framework membranes. Nevertheless, realizing three-dimensional orientation control remains a challenging issue. In this study, well-intergrown NH2-UiO-66 membranes with both (111) out-of-plane and regional in-plane orientations were prepared by combining oriented deposition of seeds and solvothermal epitaxial growth. Dynamic air–liquid interface-assisted self-assembly method was employed to organize uniform octahedral-shaped NH2-UiO-66 seeds into closely packed monolayers with (111) out-of-plane and regional in-plane orientations, whereas the use of ZrS2 as the zirconium precursor during the solvothermal epitaxial growth was found indispensible for sealing the intercrystalline gaps while preserving the preferred orientation inherited from seed layers. In addition, compared with solvothermal heating, employing microwave heating led to poor intergrowth between neighboring NH2-UiO-66 crystals because of a lower dielectric loss factor of the reaction medium. Gas permeation results indicated that the prepared NH2-UiO-66 membranes exhibited H2/CO2 selectivity up to 5.5 times higher than their counterparts with random and/or mere out-of-plane orientations as well as H2 permeability 14.5 times higher than NH2-MIL-125(Ti) membranes with mere out-of-plane orientation under similar operating conditions.
研究领域:
材料科学
·
化学工程
·
膜技术
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2020
·
IF 7.183
Xiaochang Cao,Haoqing Xu,Songlin Dong,Jiayou Xu,Zhihua Qiao,Song Zhao,Jixiao Wang,Zhi Wang
In this work, we proposed a simple method to prepare high-performance and pressure-resistant mixed matrix membranes (MMMs) for CO 2 /H 2 separation. The groups or segments of poly-(vinylamine) (PVAm) were used to modify covalent organic frameworks (COFs), and COFs with similar frameworks but different surfaces were obtained. Then, modified COFs were mixed with PVAm matrix and used to coat the modified-polysulfone (mPSf) to prepare MMMs for CO 2 /H 2 separation. Modified COFs and the PVAm matrix were highly compatible because COF surfaces possessed the same groups or segments as PVAm. Meanwhile, in the coating solution, COF surfaces were found to induce penetration of PVAm molecules into COF pores, narrowing the pore size of the COFs and providing an amino environment for CO 2 preferential absorption and transport. The penetration degree was affected by the hydrogen bond between COF surfaces and the PVAm molecules. In addition, the incorporated COFs effectively restricted the mobility of the PVAm matrix, increasing the pressure resistance for MMMs under high pressure. In the gas permeation test, the optimal MMMs could achieve a CO 2 permeance of 957 GPU and a CO 2 /H 2 selectivity of 17.1 at 2.0 MPa because of the high compatibility and size of the channels (0.94 nm).
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
MACROMOLECULES
·
2024
·
IF 5.1
Yu Zhang,Feng Zhang,Shuqi Liu,Lele Guo,Zhenggong Wang,Jian Jin
High-performance polymer-based H2/CO2 separation membranes are attractive for sustainable blue hydrogen production. However, achieving high-flux separation remains a challenge, as H2 and CO2 have similar diffusion rates within the polymer. In this work, hydrogen-bonded polyamide (PA) network membranes are synthesized through interfacial polymerization involving Tröger’s base diamine (TBDA) and 1,3,5-benzenetricarbonyl trichloride, aiming to enhance the efficiency of H2/CO2 separation. Incorporating the contorted TBDA unit into the PA structure enhances microporosity, which, in turn, boosts the H2 permeance of the PA membrane. Notably, the presence of numerous intermolecular hydrogen bonds between N atoms in the TBDA and H atoms in the amide groups helps to restrict the pore size further, thereby improving the H2/CO2 selectivity of the membrane. The resulting PA membrane demonstrates an outstanding H2/CO2 selectivity of 23.5, coupled with a high H2 permeance of 160 gas permeation unit (GPU), significantly exceeding the current upper bound. Additionally, our PA membranes maintain a stable H2/CO2 selectivity of approximately 21.5 and a H2 permeance of around 160 GPU over 100 h, indicating excellent long-term stability. These findings suggest that the development of such advanced polymer membranes could pave the way for more efficient and sustainable blue hydrogen production, overcoming existing limitations in gas separation technologies.
研究领域:
材料科学
·
化学工程
·
可持续能源
✓ 已验证
产品关联
DOI
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
·
2023
·
IF 5.7
Meng Chen,Huawei Fang,Chao Wang,Jixiang Xu,Lei Wang
Background Solar-driven water splitting is regarded as one promising green way to produce H 2 . Photo-reduction of hexavalent chromium (Cr(Ⅵ)) to hypotoxic Cr(III) can control the Cr(VI)-induced pollution. A key in these processes is to develop a photocatalyst with high specific surface area, good light absorption and efficient charge carrier separation. Methods A Co-encapsulated N-doped carbon (Co@NC) was prepared by pyrolysis ZIF-8@ZIF-67 precursor to modify CdSe quantum dots (QDs). The obtained catalyst was used to reduce Cr(Ⅵ) and split water under visible light irradiation. Significant findings Modification CdSe with Co@NC made obtained Co@NC/CdSe possessing enhanced visible-light absorption and photoexcited charge separation. The optimal 2%Co@NC/CdSe exhibited the excellent Cr(Ⅵ) reduction performance with a rate constant of 0.28 min –1 in the absence of sacrificial agent, as well as high H 2 evolution rate of 6.48 mmol g –1 h –1 in 10% lactic acid solution. The H 2 O 2 and electrons were the active species to reduce Cr(VI). This work gives a beneficial insight for improving the photocatalytic activity of QDs.
研究领域:
环境科学
·
材料科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Experimental Nanoscience
·
2022
·
IF 2.024
Zhen-Hong He,Yuan-Yuan Wei,Na Li,Yong-Chang Sun,Shao-Yan Yang,Kuan Wang,Weitao Wang,Xiaoxue Ma,Zhao-Tie Liu
Chemical utilization of CO2 is one of the fundamental strategies to synthesize value-added chemicals and reduce the CO2 emission. N-formyl-1,2,3,4-tetrahydroisoquinoline derivatives (FTHIQs) are important chemicals for the synthesis of medical intermediates and alkaloids. N-formylation of isoquinoline derivatives (IQs) with CO2 is an ideal protocol to synthesize the FTHIQs and utilize the CO2 source. In the present work, we prepared a heterogeneous Ru/ZIF-8 catalyst with a Ru loading of 2 wt% by a simple impregnation method and assessed its performances in the N-formylation of IQs and CO2 with H2. The Ru/ZIF-8 catalyst offered high IQ conversion of 98% and FTHIQ selectivity of 93% in the reaction under relatively mild conditions (150 °C, 2 MPa CO2, and 6 MPa H2). The catalyst possessed good universality and reusability, showing a potential in wide application of N-formylation of highly unsaturated nitrogen-containing isoquinolines.
研究领域:
催化
·
绿色化学
·
有机合成
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2012
·
IF 4.951
Jing Yang,Ligang Feng,Fengzhan Si,Yuwei Zhang,Changpeng Liu,Wei Xing,Kunqi Wang
H 2 -mesoporphyrin IX and Zn-mesoporphyrin IX have been investigated as sensitizers for the titanium dioxide (TiO 2 ) film electrode to construct a new two-compartment photoelectrochemical biofuel cell (PEBFC). The PEBFC can convert the light and chemical energy to electricity by consuming photons and oxidizing glucose. The two sensitizers are similar with two carboxyl anchoring groups, except that the central hydrogen atoms in the H 2 -mesoporphyrin IX are replaced by zinc. To determine how cell performance is affected by the sensitizer, we analyze the photochemical and photoelectrochemical properties of the two sensitizers by physical characterization and photoelectrochemical experiments. The UV–Vis absorption spectra and X-ray photoelectron spectra (XPS) indicate that the interactions between the sensitizer and TiO 2 decrease in the order of H 2 -mesoporphyrin IX > Zn-mesoporphyrin IX. The interactions are also determined by Fourier transform infrared (FTIR) spectra which indicate that the two sensitizers are adsorbed on the TiO 2 film through the carboxyl groups. The photovoltaic characteristics show the Zn-mesoporphyrin IX is less effective in comparison with the H 2 -mesoporphyrin IX, since the Zn-mesoporphyrin IX enhances the back electron-transfer process, producing lower IPCE and current. These results reveal that the H 2 -mesoporphyrin IX is a more efficient sensitizer compared with the Zn-mesoporphyrin IX for the PEBFC.
研究领域:
生物化学
·
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2019
·
IF 6.35
Shuzhen Lv,Kangyao Zhang,Ling Zhu,Dianping Tang,Reinhard Niessner,Dietmar Knopp
With the introduction of gas-based contactless electrochemical biosensors lies the prospects of separating the sensing interface from the bioassembly platform, enhancing stability, and exploring signal transduction mechanism, all intimately linking to development of immunoassay. Herein, we report on a H2-based electrochemical biosensor whose signals derived from the chemical signal transduction between a H2 and Pd nanowires@ZIF-67 (ZIF: Zeolitic Imidazolate Frameworks) bilayered sensing interface for immunoassay. Dendritic Pt nanoparticles (DPNs) conjugated on the detection antibody were introduced on the interface of a magnetic microsphere according to an immune sandwich assembly between the antigen and antibody. H2 as a bridge originates from DPNs catalyzing NH3BH3 and links biological signals to electrical signals by reacting with Pd nanowires. Nevertheless, the response of Pd nanowires being extremely effected by O2 in air due to the competitive adsorption on the surface of Pd nanostructures as well as the reaction between chemisorbed O (Pd–O) and adsorbed dihydrogen lead to a decrease in H absorption into PdHx and poor sensing responses under low target concentration. Porous ZIF-67 (window aperture 0.331 nm) as a molecular sieve self-assembling on the surface of the Pd nanowires film could easily permeate H2 (kinetic diameter of 0.289 nm), while interferential O2 (kinetic diameter of 0.346 nm) has difficultly passing through the ZIF-67 layer to contact Pd nanowires and achieves a response of a lower concentration target as well as faster response rate. Under optimal conditions, H2-based electrochemical biosensors exhibit great response toward target alpha-fetoprotein (AFP) within a dynamic working range of 0.1–50 ng mL–1 at a detection limit of 0.04 ng mL–1. Our strategy provides a reusable sensing interface, high specificity, and acceptable accuracy for the immunoassay. In addition, it also expands a promising platform for application as a molecular sieve in electrochemical biosensors.
研究领域:
生物传感器
·
纳米技术
·
分析化学
·
材料科学
·
生物医学工程
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Peng Li,Chao Ma,Ning Li,Chi Tang,Zhaolin Lv,Zhenjie Gu,Zhihua Qiao,Chongli Zhong
Metal-organic framework (MOF) membranes have demonstrated significant potential in replacing traditional polymer membranes for gas separation. However, synergistically enhancing gas permeance and selectivity remains challenging in MOF membrane design, particularly when framework pore apertures surpass gas kinetic diameters. Here, an innovative strategy is reported for engineering ultrathin ZIF-8 membranes with chemical adsorption sites via polymer bidirectional induction. The polyethyleneimine (PEI)-Zn 2+ interface layer facilitated the formation of ultrathin ZIF-8 membranes (~78.4 nm) by guiding small-sized crystal growth. Meanwhile, the competitive coordination of PEI with 2-methylimidazole induced the pendant of partially coordinated ligands in the ZIF-8 cavity to form chemisorption sites. This structural alteration enabled the in-situ chemical adsorption of CO 2 in the cavity of ZIF-8, thus contracting the window apertures and enhancing the molecular sieving efficiency. As a result, the ultrathin ZIF-8 membrane exhibited an excellent H 2 /CO 2 ideal selectivity of 34.2 with a remarkable H 2 permeance of 7143.6 GPU in single-gas tests, outperforming other reported ZIF-8 membranes. During mixed-gas H 2 /CO 2 testing, the in situ structural changes demonstrated robust pressure-performance stability and long-term gas separation capability. This work advances the development of ZIF-8 membranes for efficient separation of H 2 /CO 2 , and offers a feasible design principle and theoretical guidance for MOF-based gas separation membranes.
研究领域:
材料科学
·
化学工程
·
膜技术
·
气体分离
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
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.
研究领域:
电化学
·
催化
·
材料科学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Nano Research
·
2020
·Vol. 13
·期 12
·3206-3211
·
IF 8.183
Zhang Meng,Hu Zheng,Gu Lin,Zhang Qinghua,Zhang Linghui,Song Qian,Zhou Wei,Hu Shi
A series of carbon-based binary single-atom catalysts of Fe and Ni coordinated by nitrogen are fabricated using a glucose-chelating method. Depending on the Ni/Fe content, they exhibit a wide-range of controllable CO/H 2 ratio from 0.14 to 10.86, which is meaningful to specific chemical processes. The durability of the catalyst is evaluated over an 8-hour period with no significant degradation of activity. The variation of the faradaic efficiency with Ni/Fe content is justified by density-functional-theory based calculation of the reaction barrier in both hydrogen evolution and CO 2 reduction reactions.
研究领域:
催化
·
电化学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2021
·Vol. 16
·期 4
·498-510
·
IF 4.204
Bo Jinxiao,Li Mei,Zhu Xinli,Ge Qingfeng,Han Jinyu,Wang Hua
The electrochemical conversion of CO 2 -H 2 O into CO-H 2 using renewable energy is a promising technique for clean syngas production. Low-cost electrocatalysts to produce tunable syngas with a potential-independent CO/H 2 ratio are highly desired. Herein, a series of N -doped carbon nanotubes encapsulating binary alloy nanoparticles (M x Ni-NCNT, M= Fe, Co) were successfully fabricated through the co-pyrolysis of mela-mine and metal precursors. The M x Ni-NCNT samples exhibited bamboo-like nanotubular structures with a large specific surface area and high degree of graphitization. Their electrocatalytic performance for syngas production can be tuned by changing the alloy compositions and modifying the electronic structure of the carbon nanotube through the encapsulated metal nanoparticles. Consequently, syngas with a wide range of CO/H 2 ratios, from 0.5:1 to 3.4:1, can be produced on M x Ni-NCNT. More importantly, stable CO/H 2 ratios of 2:1 and 1.5:1, corresponding to the ratio to produce biofuels by syngas fermentation, could be realized on Co 1 Ni-NCNT and Co 2 Ni-NCNT, respectively, over a potential window of −0.8 to −1.2 V versus the reversible hydrogen electrode. Our work provides an approach to develop low-cost and potential-independent electrocatalysts to effectively produce syngas with an adjustable CO/H 2 ratio from electrochemical CO 2 reduction.
研究领域:
材料科学
·
电化学
·
可再生能源
·
催化
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Caiyun Xu,Kaijie Li,Hongbo Yu,Mingxi Liu,Shenghu Zhou
In this work, Pt nanoparticles encapsulated hollow porous silica nanoreactors (Pt@HPSNs) was synthesized in one-pot by a reverse microemulsion system, and they exhibit good catalytic efficiency and stability for semihydrogenations of alkynes . The key design concept is to form Pt hydroxide nanoparticles mixed poly(ethyleneimine) nano-aggregates in water droplets, which further functions as seeds for silica deposition and the void templates to form the central voids. The Pt@HPSNs illustrate a wide adaptability for semihydrogenations of a series of terminal alkynes to the corresponding alkenes at mild reaction conditions, and demonstrate high yields of styrene for semihydrogenation of phenylacetylene, showing good catalytic efficiency for hydrogenation of phenylacetylene to styrene at atmospheric H 2 pressure. The enhanced catalytic performance of Pt@HPSNs are ascribed to their hollow porous nanostructures , where the confinement of Pt nanoparticles in voids increase the structural stability and the confinement effect may increase the collision of reactants and Pt, resulting in improved catalytic efficiency.
研究领域:
催化
·
纳米技术
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）