CHINESE JOURNAL OF CATALYSIS
·
2021
·Vol. 42
·期 6
·1024-1029
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IF 8.271
Ting Wang,Shaoxiong Li,Bingling He,Xiaojuan Zhu,Yonglan Luo,Qian Liu,Tingshuai Li,Siyu Lu,Chen Ye,Abdullah M. Asiri,Xuping Sun
The typical Haber technical process for industrial NH 3 production involves plenty of energy-consumption and large quantities of greenhouse gas emission . In contrast, electrochemical N 2 reduction proffers environment-friendly and energy-efficient avenues to synthesize NH 3 at mild conditions but demands efficient electrocatalysts for the N 2 reduction reaction (NRR). Herein we report for the first time that commercial indium-tin oxide glass (ITO/G) can be used as a catalyst electrode toward artificial N 2 fixation, as it demonstrates excellent selectivity at mild conditions. Such ITO/G delivers excellent NRR performance with a NH 3 yield of 1.06 × 10 −10 mol s −1 cm −2 and a faradaic efficiency of 6.17% at –0.40 V versus the reversible hydrogen electrode (RHE) in 0.5 M LiClO 4 . Furthermore, the ITO/G also possesses good electrochemical stability and durability. Finally, the possible reaction mechanism for the NRR on the ITO catalysts was explored using first-principles calculations.
研究领域:
电化学
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材料科学
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可持续能源
·
催化
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2024
·Vol. 40
·期 6
·1192-1200
·
IF 3.1
Huang Yitong,Wang Yaquan,Liu Wenrong,Bu Lingzhen,Qu Liping,Chu Kailiang,Guo Niandong,Zhang Xian,Su Xuemei,Li Yaoning,Sang Juncai
A series of low silica X zeolites (LSX) was synthesized through a seed-iteration approach, based on the seed addition strategy, and then loaded with lithium ions by an ion exchanging method to obtain high N 2 adsorption capacity. These zeolites were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared spectra (FTIR), thermogravimetric analysis (TGA) and N 2 adsorption-desorption, and the adsorption capacity of N 2 and O 2 was evaluated by the vacuum pressure swing adsorption (VPSA) operation. The results showed that the nucleation period of the synthetic process could be effectively shortened by adding seed; as the seed iterations increased, the specific surface area and pore volume of the zeolites increased; the higher specific surface area and the pore volume, the higher the extent of the N 2 adsorption capacity, with the maximum reaching 28.05 cm 3 /g. However, there were no significant differences in the adsorbed capacity of O 2 by each sample. Therefore, the N 2 /O 2 separation factor also increased gradually with iterations, with the maximum up to 6.61.
研究领域:
材料科学
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化学工程
·
吸附技术
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AICHE JOURNAL
·
2023
·Vol. 69
·期 6
·e18079
·
IF 3.7
Feifei Zhang,Hua Shang,Bolun Zhai,Xiaomin Li,Yingying Zhang,Xiaoqing Wang,Jinping Li,Jiangfeng Yang
A robust aluminum-based metal–organic framework (Al-MOF) MIL-120Al with 1D rhombic ultra-microporous was reported. The nonpolar porous walls composed of para-benzene rings with a comparable pore size to the kinetic diameter of methane allow it to exhibit a novel thermodynamic-kinetic synergistic separation of CH 4 /N 2 mixtures. The CH 4 adsorption capacity was as high as 33.7 cm 3 /g (298 K, 1 bar), which is the highest uptake value among the Al-MOFs reported to date. The diffusion rates of CH 4 were faster than N 2 in this structure as confirmed by time-dependent kinetic adsorption profiles. Breakthrough experiments confirm that this MOF can completely separate the CH 4 /N 2 mixture and the separation performance is not affected in the presence of H 2 O. Theoretical calculations reveal that pore centers with more energetically-favorable binding sites for CH 4 than N 2 . The results of pressure swing adsorption (PSA) simulations indicate that MIL-120Al is a potential candidate for selective capture coal-mine methane.
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MOLECULES
·
2023
·Vol. 28
·期 24
·8013
·
IF 4.6
Yuzhou Xia,Xinghe Xia,Shuying Zhu,Ruowen Liang,Guiyang Yan,Feng Chen,Xuxu Wang
Visible-light-driven N2reduction into NH3in pure H2O provides an energy-saving alternative to the Haber–Bosch process for ammonia synthesizing. However, the thermodynamic stability of N≡N and low water solubility of N2remain the key bottlenecks. Here, we propose a solution by developing a WO3−xhollow sphere with oxygen vacancies. Experimental analysis reveals that the hollow sphere structure greatly promotes the enrichment of N2molecules in the inner cavity and facilitates the chemisorption of N2onto WO3−x-HS. The outer layer’s thin shell facilitates the photogenerated charge transfer and the full exposure of O vacancies as active sites. O vacancies exposed on the surface accelerate the activation of N≡N triple bonds. As such, the optimized catalyst shows a NH3generation rate of 140.08 μmol g−1h−1, which is 7.94 times higher than the counterpart WO3-bulk.Keywords:WO3;hollow sphere;O defect;N2reduction;photocatalysis
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Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 15
·4519-4525
·
IF 7
Chaoran Wang,Xiao Li,Shiyue Liu,Tingting Wang,Puxu Liu,Xiaowei Song,Zhiqiang Liang
Silicoaluminophosphate (SAPO) zeolites with small pores (8-ring window), such as SAPO-34, SAPO-17, and SAPO-RHO, have attracted a lot of attention due to their unique structural features, and their applications in the field of small-molecule gas adsorption and separation. However, the fast, efficient and green synthesis of SAPO zeolites remains a great challenge. In this work, SAPO-17 zeolites were synthesized within 1 min for the first time by a seed-assisted microwave method, and the resulting samples possessed excellent performance in the application of CO2 adsorption and separation for flue gas and natural gas. The microwave-assisted route can shorten the crystallization time of traditional hydrothermal methods from a few hours to 30 min. Furthermore, the crystallization time could be drastically shortened to 1 min with the addition of seeds, which represents the shortest time for the preparation of a SAPO-17 zeolite up to now. SAPO-17 synthesized within 1 min (SAPO-17-S-1) possessed the smallest crystal size, and the largest micropore volume and specific surface area among all the samples, which enhanced mass transfer and exposed more active sites, and thus it possessed prominent performance for CO2 adsorption (3.47 mmol g−1 at 273 K and 1 bar) and gas separation. At 298 K and 100 kPa, SAPO-17-S-1 exhibited the highest gas selectivity for CO2/N2 (276) and CO2/CH4 (63) over the other samples, which were synthesized in a relatively long time. Transient binary breakthrough experiments on SAPO-17-S-1 further verified the highly-efficient gas separation performance. This work proposes a green and ultrafast strategy for the synthesis of SAPO-17 zeolites with highly selective CO2 adsorption over N2 and CH4.
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MACROMOLECULES
·
2022
·
IF 6.057
Wenwen Zhao,Wenqiang Ma,Shuangping Xu,Xintian Wang,Hongge Jia,Jingyu Xu,Mingyu Zhang,Yanqing Qu,Jiao Liu
Oxygen/nitrogen (O2/N2) permselective membranes are widely used in both industrial and medical applications. Polysiloxane is one of the most important membrane materials with high oxygen permeability, but its poor capacities for gas separation and membrane formation limit its practical use. In this study, a soluble imide-bridged polypentamethyltrisiloxane (IBPPMS) with a high molecular weight (Mn = 8.91 × 104) was designed and synthesized via a hydrosilylation reaction between polypentamethyltrisiloxane (PPMS) and N,N′-bis(3-allyl)pyromellitic diimide (DAI) in NMP under Karstedt’s catalysis. The ladder-like structure of sample was analyzed and determined through infrared spectroscopy (IR), nuclear magnetic resonance spectroscopy (1H NMR and 29Si NMR), and gel permeation chromatography (GPC). The IBPPMS membrane displays excellent thermal resistance. Furthermore, its O2 permeation performance achieves 47.1 barrer, and its separation factor reaches 7.11 with a feeding proportion of 50% each for O2/N2, exceeding the 2008 Roberson upper bound. Thus, it appears that membranes can achieve high selectivity and permeability as well as exhibit desirable thermal properties and sufficient stability when separating numerous industrial significant gas mixtures. The discovery of trapezoidal structural backbone of this polymer materials substantially affects their separation properties and sustained performances.
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JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Li Yin,Dongfeng Li,Hongxia Guo,Shuai Wang,Tiexin Zhang,Yunling Liu,Fangyuan Gai,Xiaogang Zhao
Incorporating functional materials into polymer precursors is an effective way to prepare carbon molecular sieve (CMS) membranes for solving the trade-off problem between permeability and selectivity of gas separation. In this work, we induced ZIF-8 nanoparticles (from 5 to 20 wt%) as a doping agent to construct a series of phenolphthalein-based cardo poly (arylene ether ketone) (PEK-C) -based hybrid carbon molecular sieve (ZCMS) membranes for CO 2 /N 2 separation via an oxidation and a carbonization process with pyrolysis temperature in the range of 500–700 °C. The carbonized ligand and metal centre of ZIF-8 offered additional pores of carbon matrix, which tailored the ultramicropores of ZCMS membranes for both excellent CO 2 permeability and selectivity. By treating with the temperature of 600 °C, ZCMS-600-15 (ZCMS membrane based on 15 wt% of ZIF-8-doped PEK-C) exhibited the highest CO 2 permeability of 8902 Barrer, which was 1.8 times higher than that of CMS-600 (CMS membrane based on naked PEK-C). ZCMS-600-15 showed an ideal CO 2 /N 2 selectivity value of 42.2, which is also higher than that of other samples, indicating that the appropriate doping amount of ZIF-8 is 15 wt% and the proper carbonization temperature is 600 °C. Moreover, among all the samples, ZCMS-600-15 also showed a superior CO 2 permeability of 8285 Barrer and the highest CO 2 /N 2 selectivity of 24.08 for an equimolar mixture of CO 2 and N 2 , far exceeding the 2008 Robeson upper bound. Therefore, our results suggest that incorporating MOFs into polymer precursors to prepare hybrid carbon molecular sieve membranes by carbonization process could solving the trade-off problem between permeability and selectivity, introducing new possibilities for industrial application.
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BIOCHEMICAL ENGINEERING JOURNAL
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2022
·
IF 4.446
Sijing Bi,Huimin Liu,Yuancai Chen,Yongyou Hu
The palladium nanoparticles (Bio-PdNPs) were in-situ biosynthesized in denitrifying sludge at three Pd loading levels, and the denitrification performance was evaluated in terms of interspecies hydrogen/electron transfer (IHT/IET) and their pathway for the first time. The results showed that high selectivity towards N 2 (76.96%, 97.10% and 99.30%) were observed when conventional denitrifying sludge was embedded with appropriate amount of Bio-PdNPs at three C/N ratios (3, 7 and 10), respectively. In-situ fermented hydrogen could be consecutively provided for IHT at low H/N ratio, avoiding the production of NH 4 + . IHT related with Pd[H] mainly catalyzed the enzymic/nonenzymic transformation of NO 2 - , NO and N 2 O, in which NO could be directly/abiotically cracked to N 2 and O 2 /H 2 O. Moreover, IET was greatly accelerated via the bounded flavin (FBcyt) and cytochrome , riboflavin , as well as electron hopping. Nevertheless, enzymatic denitrification was depressed with excess Bio-PdNPs (Bio-PdNPs-10). This study shed light on IET/IHT and denitrification pathway in Bio-PdNPs-mediated denitrification system, and provided basis for engineering practice.
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Nano Energy
·
2021
·
IF 17.881
Cheng Du,Chenglong Qiu,Zhongying Fang,Ping Li,Yijing Gao,Jianguo Wang,Wei Chen
Electrocatalytic nitrogen reduction reaction (NRR), which can produce ammonia from N 2 and H 2 O under ambient conditions, has emerged as a promising sustainable alternative to the Haber-Bosch (H-B) process. However, their unsatisfied conversion efficiency and selectivity severely restrict the real utilization of NRR, owing to the stubborn triple bond in the N 2 molecule and the competitive hydrogen evolution reaction (HER). Here, inspired from the local microenvironment of the nitrogenase, we report for the first time a facile and general strategy to boost the NRR selectivity and activity through the self-assembled monolayer (SAM) of hexanethiol (HEX) on a series of metal electrocatalysts (Cu, Au, Pt, Pd and Ni). Molecular dynamics (MD) simulations suggest that the HEX SAM provides a hydrophobic microenvironment to impede the diffusion and adsorption of water molecules and promote that of N 2 molecules, thus inhibiting HER and simultaneously improving the NRR performance. Notably, among all the prepared samples, the highest Faradic efficiency (FE) of 50.5% is achieved on Cu-HEX with NH 3 formation rate (R) of 1.2 μg h −1 cm −2 . Remarkably, for the HER-favored Pt catalyst, the highest R of 26.4 μg h −1 cm −2 is also achieved on Pt-HEX with FE of 1.8% under 1 cm 2 of electrode area. The present strategy not only represents a general diffusion-controlled method to engineer high-performance NRR electrocatalysts, but also provides a new insight into the effect of surface chemistry of catalysts on the NRR process and kinetics.
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Journal of Environmental Sciences
·
2023
·
IF 6.9
Junying Yi,Yuli Chen,Dongze Lai,Bihong Lv,Xiaomin Wu,Guohua Jing
Bi 2 O 3 catalyst with Bi-O bond crystal structure has more active sites, which shows better CO 2 catalytic performance than pure Bi catalysts in many catalytic reactions. How to strengthen the Bi-O bond in Bi 2 O 3 to obtain higher selectivity and catalytic activity is a problem worthy of consideration. Here, we develop a N 2 pre-reduced spherical Bi 2 O 3 /ATO catalyst that has a high formate Faradaic efficiency of 92.7%, which is superior to the existing tin oxide catalyst. Detailed electrocatalytic analysis shows that N 2 pre-reduction and spherical structure are helpful for Sn to stabilize the oxidation state of Bi, thus retaining part of the Bi-O structure. The existence of the Bi-O structure can reduce the energy barrier of the CO 2 production *OCHO reaction and promote the reaction rate of the CO 2 -*OCHO-HCOOH path, thus promoting the formation of formate.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xuerui Bai,Maiqian Nie,Zhenjun Diwu,Lei Wang,Hongyun Nie,Yan Wang,Qiuyue Yin,Bo Zhang
2-Hydroxymuconic semialdehyde (2-HMS) is a useful intermediate in organic synthesis, but there are few reports for its preparation. 2-HMS accumulates in phenol-containing wastewater treated with Pseudomonas stutzeri N2. This work has studied the extraction of 2-HMS so that the phenolic wastes of high concentration may be used to produce 2-HMS. When 4.25 mmol/L phenol was degraded by Pseudomonas stutzeri N2, the accumulated 2-HMS can reach 3.79 ± 0.08 mmol/L within 30 h. A saturated solution of NaHSO 3 was added into the 2-HMS culture, and white rod-like precipitates formed gradually. Through SEM, XRD and FT-IR, the precipitates were identified as monoclinic hexagonal crystals of α-hydroxy sulfonate sodium with high purity. In the presence of NaOH, α-hydroxy sulfonate sodium could be reduced to the desired 2-HMS product. The optimized conditions were characterized to be 3 mol/L NaOH solution, 5 min and 50 °C. The conversion rate of α-hydroxy sulfonate sodium was up to 87.3 ± 0.2%, and 0.42 ± 0.02 mmol/L 2-HMS were obtained.
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ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Zhen Liu,Mengzhao Zhang,Huining Wang,Danyun Cang,Xuqiang Ji,Bingping Liu,Wenrong Yang,Da Li,Jingquan Liu
In industry, ammonia (NH3) is currently produced by Haber–Bosch technology, which suffers from the drawbacks of high energy consumption and CO2 emission. Artificial N2 fixation in aqueous solution under ambient conditions has been recently pushed forward by developing electrocatalysts with high efficiency and high selectivity for NH3 production. Herein, we demonstrate that defective carbon-doped boron nitride nanosheets (C-BN) show excellent electrocatalytic activity and durability in N2 fixation. To be used as a cathode catalyst, C-BN achieves an NH3 production rate of 36.7 μg h–1 mgcat–1 at −0.55 V vs a reversible hydrogen electrode (RHE), which is much higher than that of the synthesized and exfoliated boron nitride nanosheets. The faradic efficiency of C-BN attains 6.51% at −0.55 V vs RHE, which indicates excellent selectivity of the N2 reduction reaction (NRR). Furthermore, the catalysts show great stability during electrolysis and recycling tests. In principle, carbon doping and the defective structure contribute to the promoted NRR performance of C-BN.
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