JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Guangmin Ren,Zehui Zhao,Zizhen Li,Zisheng Zhang,Xiangchao Meng
Herein, we applied a rapid Joule heating method to form oxygen vacancies and further induced the deposition of Ru clusters onto BiVO 4 . The rapid Joule heating method fabricated oxygen vacancy on BiVO 4 , resulting in the formation of electron-rich active Ru sites and unsaturated V sites. The pristine BiVO 4 was almost no activity in photocatalytic ammonia synthesis. The photocatalytic production rate of ammonia was increased to 3.88 μmol g - 1 h -1 after the formation of oxygen vacancies, and further increased to 16.57 μmol g -1 h -1 with Ru clusters loaded on BiVO 4 . It was indicated that unsaturated V sites near the oxygen vacancy and Ru clusters might act as the reactive sites for N 2 adsorption and activation. And the strong metal-support interactions between Ru and BiVO 4 resulted in charge redistribution between Ru clusters and BiVO 4 supports, thus reducing energy barrier of the rate-determining step for the N 2 hydrogenation. Furthermore, DFT confirmed that associative alternating pathway was suitable for this process.
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AICHE JOURNAL
·
2020
·Vol. 67
·期 4
·e17114
·
IF 3.519
Ihtisham Ul Haq,Tao Wang,Ao-Shuai Zhang,Heng Mao,Rehan Khan,Li-Hao Xu,Zhi-Ping Zhao
1,3-Butadiene (BD) is a petrochemical-based volatile organic compound, extensively used for the manufacture of synthetic rubber. There is no method reported for its recovery from nitrogen mixture. Herein, for the first time, BD is efficiently recovered by gas separation through facile and novel mixed-metal ZIF-8 based mixed matrix membranes (MMMs). Addition of Ni-ZIF-8 nanoparticles in PDMS matrix, significantly improved the penetrant-membrane interactions and the solution-diffusion properties of BD. Positron annihilation lifetime spectroscopy analysis showed that the well dispersion of Ni-ZIF-8 in PDMS enhanced the free volume of membrane and created efficient continuous paths for BD diffusion. Then, 15 wt% Ni-ZIF-8 MMM exhibited the BD permeance of 323 GPU and the BD/N 2 ideal selectivity of 19.5, which were 60 and 81% higher than pure PDMS membrane, respectively. The simultaneous enhancement of BD permeance and BD/N 2 ideal selectivity indicated that Ni-ZIF-8 was an effective filler applied in MMMs for efficient BD recovery.
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JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 55
·期 26
·12041-12052
·
IF 3.553
Yi Xuerui,He Xiaobo,Yin Fengxiang,Yang Tong,Chen Biaohua,Li Guoru
The global NH 3 production is dominated by Haber–Bosch process, requiring high temperature and pressure. Electrochemical N 2 reduction reaction (NRR) under ambient conditions is a greener path for artificial N 2 fixation to NH 3 but calling for efficient catalyst to increase activity and selectivity. Herein, we report the iron-based metal–organic frameworks (MOFs), i.e., MIL-88B–Fe and amine-functionalized MIL-88B–Fe (NH 2 –MIL-88B–Fe) as efficient catalysts for electrochemical NRR under ambient temperature and pressure in neutral electrolyte. NH 2 –MIL-88B–Fe shows higher NH 3 yield rate of 1.205 × 10 –10 mol s −1 cm −2 than MIL-88B–Fe (3.575 × 10 –11 mol s −1 cm −2 ). Furthermore, NH 2 –MIL-88B–Fe exhibits the highest Faradaic efficiency of 12.45% at 0.05 V versus RHE. The control experiments prove that NH 3 is produced through electrocatalytic NRR. This work may trigger the interest of using MOFs as highly efficient catalysts for electrochemical NH 3 production.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Yifan Li,Yaqin Hou,Yongzhao Zhang,Yatao Yang,Zhanggen Huang
Surface interface regulation is an important research content in the field of heterogeneous catalysis. To improve the interface interaction between the active component and matrix, tremendous efforts have been dedicated to tailoring the morphology, size, and structure of composite catalysts. In this work, we report a confinement strategy to synthesize a series of core-shell catalysts loaded with metal oxides on titania nanotubes (TNTs), which were applied to the selective catalytic reduction of NO x with ammonia. Interestingly, the core-shell catalyst with confinement of TNTs exhibited the remarkable activity at low temperature region, N 2 selectivity and sulfur tolerance. Benefiting from the superior interfacial confinement characteristic of TNTs and Fe 2 O 3 , strong component interactions, the surface acid sites and strong oxidizability of MnO x were properly regulated, thus obtained the outstanding activity, N 2 selectivity and provide chemical protection to effectively prevent SO 2 poisoning. As far as the reaction mechanism, we found that the adsorption and reactivity of Lewis acid sites were the dominant factors affecting the activity in the NH 3 -SCR process by in situ DRIFT spectra. In general, our work provides an innovative strategy for constructing an TNTs-enwrapped nanocomposite with nano-confinement and core-shell structure to improve the low temperature SCR process.
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Catalysis Science & Technology
·
2019
·Vol. 9
·期 5
·1208-1214
·
IF 5.726
Linchuan Cong,Zhuochen Yu,Fangbing Liu,Weimin Huang
Ammonia is an important precursor of fertilizers and nitrogen compounds, and it is also a potential energy storage medium and alternative fuel for vehicles. The main ammonia production process is the Haber–Bosch process, which is energy- and capital-intensive. Therefore, it is crucial to find an alternative method for the synthesis of ammonia. In this paper, we reported a new non-noble metal N-doped nanocarbon/Fe3C nanoparticle catalyst (NCF) for the electrochemical synthesis of ammonia, yielding an NH3 production rate of 15.804 μg h−1 mgcat.−1 and Faradic efficiency (FE) as high as 2.72% at −0.4 V vs. RHE at room temperature and ambient pressure in 0.1 M KOH electrolyte. We believe that this work will provide a new opportunity to design a new non-noble metal catalyst for the nitrogen reduction reaction (NRR) and also open a new route to solve the global energy and ecological crisis.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2018
·
IF 3.779
Shun Dong,Wenzheng Zhang,Ping Hu,Yumin Zhang,Jiecai Han,Xiaoguang Luo
Nitrogen-doped SiC microparticles (SiCp) and SiC nanowries (SiCNWs) with different nitrogen contents were successfully synthesized by a simple and effective method, in which SiCp and SiCNWs were directly annealed in N 2 at 1500 °C with different holding times to adjust the contents of nitrogen for the first time. The nitrogen content of N-doped SiCp and SiCNWs increased with holding time, from 2.91 at.% and 3.05 at.% for 1 h to 5.05 at.% and 5.25 at.% for 4 h. The size of N-doped SiCp and SiCNWs was larger than that of pristine SiCp and SiCNWs, while the size tended to increase firstly and then decrease. The results of dielectric parameters showed that both real part ε′ and imaginary part ε ″ of permittivity of the samples increased greatly with increasing N contents in most frequency range, while two opposing trends for nitrogen content dependent microwave absorption property of N-doped SiCp and SiCNWs were observed. The electromagnetic (EM) wave absorption capability of N-doped SiCp was significantly improved with increasing nitrogen content compared with fully permeable wave pristine SiCp, and the minimum reflection loss (RL m ) and maximum effective absorption bandwidth (EAB) could be up to −33.5 dB and 4.4 GHz, respectively. The EM wave absorption performance of N-doped SiCNWs exhibited a decreasing tendency with increasing nitrogen content, and the RL m was decreased from −57 dB for pristine SiCNWs, to −51.2 dB for SiCNWs with 3.05 at.% N, and to −29.3 dB for SiCNWs with 5.25 at.% N. Moreover, if the experimental process in present study was decomposed into heat-treatment and N-doping, the heat-treatment played extremely negative effect on the EM wave absorption performance of samples, while N-doping still had positive impact on the EM wave absorption performance. It is believed that the current work will provide a new insight into the fabrication of SiC materials with fascinating properties by doping.
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FLUID PHASE EQUILIBRIA
·
2017
·
IF 2.473
Qiaoyan Shang,Shuqian Xia,GuanWei Cui,Bo Tang,Peisheng Ma
Interfacial tension (IFT) is crucial for characterizing the phase and interphase behavior in the enhanced oil recovery (EOR) process. CO 2 and N 2 are commonly used as injection gases in the EOR process. In this work, an experimental apparatus using the pendent drop method was adopted to measure IFTs for the EOR process with different injection gases, temperatures (40.0–120.0 °C) and pressures (0.22–17.32 MPa). The relative Gibbs adsorption isotherm ( Γ ij ) of a species i on species j were calculated by the experimental IFTs. Theoretically, new correlations were proposed to predict paraffin IFTs for pure CO 2 and mixture gas (CO 2 + N 2 ) injection. A total of 561 and 268 experimental IFTs were used to derive the correlations for pure CO 2 and mixture gas injection, respectively. The square of correlation coefficient ( R 2 ), root mean square error ( RMSE ) and average absolute relative deviations ( AARD ) for pure CO 2 were 0.9884, 0.58 and 5.45%, respectively. For the mixture gas injection, the R 2 , RMSE and AARD of the correlation were 0.9851, 0.57 and 4.47%, respectively.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Chujie Zhang,Yugao Wang,Jiaxin Jing,Jinping Li,Jiangfeng Yang
Coal-based porous carbon usually has broad pore size distribution, and it remains a major challenge for achieving controllable and optimized pore size distributions in the ultramicroporous (<0.7 nm) range. In this work, coal-derived humic acid-based carbons (HACs) were successfully synthesized by in-situ ionic activation, which consumed much less KOH than the traditional KOH activation method, demonstrating environmentally friendly advantages. The prepared HACs were characterized of the concentrated ultramicroporous pore size distribution. Importantly, ultramicroporous pore size of HACs could be controlled at the sub-angstrom level by slightly adjusting the KOH amount. Dynamic breakthrough experiments and PSA process simulations strongly demonstrated the superior and applicable separation performance of HACs for CH 4 /N 2 mixtures. The investigation extends the application of in-situ ionic activation in coal-based materials and provides a cheap, green, and efficient coal-based adsorbent for low-concentration coalbed methane enrichment.
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POLYMER ENGINEERING AND SCIENCE
·
2018
·
IF 1.551
Tengyang Zhu,Xing Yang,Yayun Zheng,Xiaoqi He,Feifei Chen,Jujie Luo
A series of poly(amide- co -poly(propylene glycol)) (PA-PPG) random copolymers with different content of PPG were designed by polycondensation reaction. These random copolymers were blended up to 60% with commercially available Pebax 2533. The blend membranes were characterized by Fourier-transform infrared (FTIR) spectroscopy, X-ray diffraction (XRD), scanning electron microscope (SEM). Gas permeation properties of these blend membranes were investigated using five single-gases (CO 2 , H 2 , O 2 , CH 4 , and N 2 ) at different temperature of 25–55°C and 1.0 atm. The impacts of content of PA-PPG with different PPG content and operating temperature on CO 2 separation properties of Pebax/PA-PPG blend membranes were studied. The results showed that CO 2 permeability gradually increased with the increasing operating temperature, whereas CO 2 permeability gradually decreased with the increase in content of PA-PPG. CO 2 /N 2 selectivity gradually increased with the increase in content of PA-PPG. In particular, Pebax/PA-PPG (50)–60% displayed excellent CO 2 and O 2 separation properties ( P CO2 = 79.7 Barrer and P O2 = 13.6 Barrer, CO 2 /N 2 = 34.7 and O 2 /N 2 = 5.9) at 25°C and 1.0 atm. POLYM. ENG. SCI., 59:E14–E23, 2019. © 2018 Society of Plastics Engineers
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DALTON TRANSACTIONS
·
2025
·
IF 3.3
Zhaojie Wang,Xinle Sun,Qinglong Liu,Caifeng Xia,Qikang Yin,Siyuan Liu,Xiaoqing Lu,Hongyu Chen
Mixed matrix membranes (MMMs), which incorporate metal-organic frameworks (MOFs) nanofillers within a polymer matrix, offer a highly promising solution for CO2 capture and separation. However, poor interfacial compatibility and filler aggregation in MMMs pose significant challenges to enhancing CO2/N2 separation performance. Here, we present a novel approach using amino ionic liquid modification to optimize MMMs, where the modified AFIL promotes the formation of ZIF-8 with well-defined facets and sharp edges, and enhances the compatibility between ZIF-8 particles and PIM-1 polymer matrix for favorable CO2 affinity and selective CO2 transport. The resulting 10 wt.% AFIL@ZIF-8/PIM-1 exhibits exceptional gas separation performance with a CO2 permeability of 7864262.2 Barrer and a CO2/N2 selectivity of 29.661.96. More importantly, the incorporation of AFIL into the ZIF-8 pores significantly enhances the thermal stability and aging resistance of AFIL@ZIF-8/PIM-1 MMMs via structural support and hydrogen bonding interactions. This work provides a practical approach to developing hybrid membranes for CO2/N2 separation, showcasing improved overall performance and strong interfacial compatibility.
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LANGMUIR
·
2012
·
IF 4.186
Qi Zhang,Guoqiang Yu,Wen-Jun Wang,Haomiao Yuan,Bo-Geng Li,Shiping Zhu
This work reports the development of a reversibly coagulatable and redispersible polystyrene latex system that can be triggered by N2/CO2. The coagulatability and redispersibility of the latexes were achieved by employing 0.9–5.6 wt % (N-amidino)dodecyl acrylamide (DAm), a reactive switchable surfactant, in an emulsion polymerization of styrene under CO2 atmosphere. The resulted latex particles were readily coagulated by N2 bubbling at 60 °C and redispersed by CO2 bubbling and ultrasonication, which switched amidine moieties between neutral and ionic states. The coagulation/redispersion processes were repeatable. The prepared latexes showed good stabilities against electrolytes, especially with higher charges.
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PROCEEDINGS OF THE COMBUSTION INSTITUTE
·
2024
·
IF 5.3
Nan Liu,Qi Chen,Xianwu Jiang,Jie Chen,Lidong Zhang,Jiaying Pan,Haiqiao Wei,Xingqian Mao
This work presents a three-stage hybrid nanosecond discharge (NSD) and direct current (DC) discharge assisted n -C 5 H 12 /O 2 /N 2 ignition with lower discharge energy and higher energy efficiency. The reaction rate coefficients between O 2 (a 1 Δ g ) and n -C 5 H 12 are updated by mass/Master equation simulation. The promotive ignition enhancement via reaction channel O 2 (a 1 Δ g ) + n -C 5 H 12 → C 5 H 10 + H 2 O 2 in the hybrid NSD/DC discharge is demonstrated. The results show that the ignition delay time of the three-stage hybrid plasma assisted ignition is 1–2 orders of magnitude shorter than that of the two-stage hybrid discharge when the reduced electric field strength in the DC discharge stage is over 10 Td. Meanwhile, the plasma-enhanced energy efficiency of three-stage hybrid discharge increases. This improved efficiency on ignition enhancement is due to the kinetic enhancement by the electronically excited species and radicals (O 2 (a 1 Δ g ), O( 1 D), N 2 (B) and O). The kinetic and thermal effects by plasma are effectively intergated to enhance ignition. However, more discharge energy deposited in the vibrationally excited states N 2 ( v ) in the two-stage hybrid discharge is less efficient on ignition enhancement due to the thermal contribution via vibrational-translational relaxation. In the aspect of NO x /N 2 O emissions, reduction efficiency of the three-stage hybrid discharge is two times higher than that of the two-stage hybrid discharge. By controlling the N/N( 2 D) production pathway e + N 2 → e + N + N( 2 D), the three-stage hybrid discharge reduces NO x and N 2 O production by 61.1 % and 90 %, respectively. The results show that the ignition delay time is non-monotonically dependent on the discharge pulse number. There exist optimal pulse number, reduced electric field and effective threshold power density of DC discharge to achieve maximum ignition enhancement and low NO x /N 2 O emissions. This study provides valuable insights into the use of NSD/DC hybrid discharge technology in advanced engines to achieve energy-efficient ignition enhancement and reduce NO x /N 2 O emissions.
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