CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yanhu Han,Zhaowei Jia,Wenxue Gong,Xuechun Wei,Yu Zhang,Mengying Tao,Yaofei Ren,Zuyi Lu,Yutong Wu,Jianhua Chen,Zhongfeng Shi,Zhenxia Zhao,Zhongxing Zhao
Developing photocatalysts with high activity and selectivity remains a significant challenge in the field of CO 2 photoreduction for producing valuable chemical or fuel products under mild conditions. Herein, photonic crystal (PC) GDY-Cu/ZnO was constructed through the in-situ induced growth of graphdiyne (GDY) on PC Cu/ZnO surface via H 2 -reduction for efficient photoreduction of CO 2 to CH 4 . With the aid of photonic crystal structure, PC GDY-Cu/ZnO exhibits a distinctive red-edge slow light region which can significantly improve the utilization efficiency of visible light and intensify photo-catalysis. Additionally, the formed all-solid-state Z-scheme system efficiently accelerates photoelectron migration, facilitating e - /h + separation. Thirdly, the surface GDY, along with the enrich oxygen vacancies generated during H 2 reduction, enhances the adsorption and activation toward CO 2 and H 2 O on PC GDY-Cu/ZnO interface. In consequence, PC GDY-Cu/ZnO demonstrates highly photocatalytic conversion of CO 2 to CH 4 , achieving a CH 4 yield of 33.67 μmol·g −1 ·h −1 with 93.3 % selectivity via slow-light-driven photocatalysis CO 2 reduction. This work provides an efficient strategy to modify ZnO for the efficient photoreduction of CO 2 to CH 4 .
研究领域:
材料科学
·
环境科学
·
化学工程
·
光催化
✓ 已验证
产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Yuanling Li,Han Yu,Jing Dai,Zhenzong Zhang,Zhichao Zhang,Hongbing Yu,Lina Liu
Non-thermal plasma (NTP) combined with catalysts supplies a potential alternative to enable the CH 4 and CO 2 conversion to work at low temperatures. In this study, different Ni/BN catalysts were synthesized using modified wetness impregnation for CH 4 and CO 2 conversion in dielectric barrier discharge (DBD) plasma. Among, BN_IPA_Ni exhibited the highest catalytic performance with a CH 4 conversion of 40.5%, a CO 2 conversion of 26.6%, a H 2 yield of 9.3% and a CO yield of 10.5%. The development of B O defects, which played a significant role in the size control of Ni particles to facilitate the dissociation of CH 4 to form H*, is the key for the high catalysis activity and selectivity in this reaction. In addition, the B O defects of BN_IPA_Ni provide an efficient route to eliminate excess CH x species, which further inhibit the nucleation growth of carbon species to inert carbon.
研究领域:
化学工程
·
催化
·
等离子体化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Communications
·
2022
·
IF 3.662
Shaocan Dong,Weiqiu Huang,Xufei Li,Xinya Wang,Baoyou Yan,Zhen Zhang,Jing Zhong
In response to global climate change, most countries have set carbon reduction targets. Mixed matrix membranes (MMMs), which combine the characteristics of inorganic nanofillers and organic matrices, have received wide attentions because of their good permeability and selective performance for the separation of CO 2 from industrial waste gases. However, the poor dispersion, compatibility and interfacial defects often lead to poor gas separation performance. In this paper, according to the dissolution-diffusion and Lewis acid-base theories, inorganic filler of amino-functionalized Bentonite (APTES-Bentonite) with -NH 2 was firstly synthesized to improve the affinity of CO 2 . Then, the dual-functionalized MMMs of APTES-Bentonite/PVDF (A-B/P MMMs) was prepared and adopted for the separation of CO 2 /CH 4 and CO 2 /N 2 , showing the increase of 87.76% and 75.31% compared to the pristine PVDF membrane, respectively. These excellent performances were attributed to the synergistic effect of APTES-Bentonite with -NH 2 groups and PVDF with -F groups, which provide a dual-functional transport pathway for CO 2 molecules due to the interactions of host-guest. Overall, the customized A-B/P MMMs offer superior CO 2 separation performance, which provides some valuable references for large-scale CO 2 capture studies.
研究领域:
材料科学
·
环境工程
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xun Wang,Zewei Liu,Jian Yan,Daofei Lv,Xin Chen,Feng Xu,Xin Zhou,Zhong Li
Developing adsorbents with exceptional CH 4 /N 2 selectivity under high pressure is a crucial commercial requirement and a significant technical challenge for the industrial high-pressure swing adsorption (HPSA) in CH 4 /N 2 separation. Only a few adsorbents were reported to address this issue. In this work, we aimed to explore two microporous MOFs with low-polarity channels for high-pressure CH 4 /N 2 separation. The Ni(BDC)(DABCO) 0.5 and its isostructural analog Ni(TMBDC)(DABCO) 0.5 were synthesized, characterized, and examined for high-pressure CH 4 /N 2 adsorption property. Due to the lower polarity channel originating from tetramethyl groups, Ni(TMBDC)(DABCO) 0.5 exhibited an exceptional methane capacity of 4.23 mmol/g and an IAST selectivity of 5.1 for the CH 4 /N 2 binary mixture at a pressure of 10 bar, surpassing the majority of previously reported materials. The GCMC simulation revealed that the low-polarity pore surfaces in both materials exhibited a higher affinity for CH 4 molecules compared to N 2 molecules, under both ambient and high pressures. The breakthrough experiments showed that Ni(TMBDC)(DABCO) 0.5 exhibited excellent dynamic separation towards CH 4 /N 2 under both 1 bar and 5 bar, indicating great potential as an emerging candidate for the recovery of CH 4 from coal-mine methane in industrial PSA processes.
研究领域:
材料科学
·
化学工程
·
吸附技术
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Qilong Peng,Yu Chen,Diyi Fang,Chuanlei Liu,Kongguo Wu,Yuxiang Chen,Hao Jiang,Yuanyuan Sun,Qiumin Wu,Di Wu,Hui Sun
ETS-4 shows great potential to achieve effective separation of challenging mixtures due to its promising tunability of pores. However, the regulation of pore size is largely limited by its low thermal stability. Here, Na-ETS-4 was synthesized by the hydrothermal method and additionally modified via ion exchange coupled with thermal treatment. Structures of all synthesized samples were examined using a variety of characterization techniques. Both adsorption equilibrium and kinetics of CO2 and CH4 on these adsorbents were evaluated on custom-made adsorption units. In addition, the mechanism of CO2 adsorption on different structural models of ETS-4 was revealed via combining with the molecular dynamics (MD) simulations. Ion exchange largely improves the thermal stability of ETS-4 and its adsorption capacities for CO2 and CH4. Ba-ETS-4-350 exhibits the largest equilibrium selectivity of 12.42 and the greatest Henry’s selectivity of 2178.51. The radial distribution function (RDF) results reveal the main adsorption sites of CO2 in different ETS-4 structures.
研究领域:
材料科学
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2016
·
IF 2.628
Qi Sun,Xianglan Xu,Honggen Peng,Xiuzhong Fang,Wenming Liu,Jiawei Ying,Fan Yu,Xiang Wang
A series of SnO 2 -based catalysts modified by Mn, Zr, Ti and Pb oxides with a Sn/M (M = Mn, Zr, Ti and Pb) molar ratio of 9/1 were prepared by a co-precipitation method and used for CH 4 and CO oxidation . The Mn 3+ , Zr 4+ , Ti 4+ and Pb 4+ cations are incorporated into the lattice of tetragonal rutile SnO 2 to form a solid solution structure. As a consequence, the surface area and thermal stability of the catalysts are improved. Moreover, the oxygen species of the modified catalysts become easier to be reduced. Therefore, the oxidation activity over the catalysts was improved, except for the one modified by Pb oxide. Manganese oxide demonstrates the best promotional effects for SnO 2 . Using an X-ray diffraction extrapolation method, the lattice capacity of SnO 2 for Mn 2 O 3 was 0.135 g Mn 2 O 3 /g SnO 2 , which indicates that to form stable solid solution, only 21% Sn 4+ cations in the lattice can be maximally replaced by Mn 3+ . If the amount of Mn 3+ cations is over the capacity, Mn 2 O 3 will be formed, which is not favorable for the activity of the catalysts. The Sn rich samples with only Sn-Mn solid solution phase show higher activity than the ones with excess Mn 2 O 3 species.
研究领域:
催化
·
材料科学
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Minmin Gou,Weifang Zhu,Yanyong Sun,Ruili Guo
Two-dimensional (2D) MOF named Cu(BPY) 2 (OTF) 2 (OTF = trifluoromethanesulfonic acid anion (CF 3 SO 3 − ), BPY = 4,4-bipyridine) possessing axial coordination anion was prepared, and then combined into Pebax® MH 1657 (Pebax) polymer to fabricate mixed matrix membranes (MMMs) for the separation of CO 2 /CH 4 gas mixtures. The inherent microporous structure and interlayer nanochannel that constructed by axial coordination anion CF 3 SO 3 − of Cu(BPY) 2 (OTF) 2 nanosheets provide selective transfer channels for CO 2 . In addition, the group that has an affinity for CO 2 , such as pyridine group and CF 3 SO 3 − anion, locating in the surface and the interlayer of Cu(BPY) 2 (OTF) 2 nanosheets, present better binding affinity and molecule selectivity for CO 2 . Owing to the synergistic effect between structure and functional groups of Cu(BPY) 2 (OTF) 2 nanosheets, the optimized CO 2 separation performance (permeability and selectivity) of the MMMs compared with that of pure Pebax were increased by 86.65% and 47.59%, respectively, under the conditions of pure gas, 0.1 MPa and 25 °C. The open narrow nanochannels and axial coordination anion in Cu(BPY) 2 (OTF) 2 nanosheet, making Cu(BPY) 2 (OTF) 2 a promising material to prepare efficient mixed matrix membrane.
研究领域:
材料科学
·
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Xiaodi Zhang,Guojie Zhang,Xiaowei Qin,Jun Liu,Guoqiang Li,Ying Xu,Yongkang Lv
A series of nitrogen doped biomass carbon catalysts were prepared through two different nitrogen doped methods by using soybean meal as the raw material, melamine as nitrogen source and KOH as the activators. The catalysts were characterized by BET, SEM , CO 2 -TPD, EA , FTIR , XPS and Raman. The catalytic performances of CH 4 –CO 2 reforming over different samples were also studied. The results show that the preparation method of the catalyst significantly affects the structural characteristics, N content and N species type of the catalyst. The characterization results also show the proportion of pyrrolic-N in the catalyst prepared by in-situ nitrogen doped method (Y-NC) is higher than that in prepared by the post-treatment method (H-NC). Pyrrole-N is more conducive to the adsorption and activation of CO 2 . So, the catalyst prepared by in-situ nitrogen doped method has good catalytic activity and stability. The conversion of CH 4 and CO 2 were respectively 40% and 65% at 900 °C after 50 h of CH 4 –CO 2 reforming reaction .
研究领域:
催化
·
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Zhihao Song,Xinrui Liu,De Ao,Zhihua Qiao,Zhi Wang,Song Zhao
Metal-organic framework glass shows great promise in gas separation applications, however, its inherent low porosity poses significant challenges to achieve the enhanced membrane permeability. In this work, we developed novel self-standing crystal-glass composite membrane via melt quenching process of porous organic cages and coordination polymer glasses. The resulting (CC3) n /( a g Zn-P-dmbIm) 1-n membranes effectively combines the high porosity of CC3 with the excellent film-forming property of Zn–P-dmbIm glass, enabling efficient CO 2 /CH 4 separation. Specifically, CO 2 molecules are preferentially adsorbed into the CC3 channels, followed by rapid permeation through the membrane, while the size exclusion restricts CH 4 molecules transport through the membranes. The obtained (CC3) 0.05 /( a g Zn-P-dmbIm) 0.95 membrane achieves a high CO 2 permeability of 9358 Barrer, a CO 2 /CH 4 selectivity of 24.2, and demonstrates 24-h operational stability. This study not only broadens the application scope of coordination polymer glasses in gas separation membranes but also provides novel insights for the design of high-performance crystal-glass composite membranes.
研究领域:
材料科学
·
膜技术
·
气体分离
·
可持续能源
·
聚合物化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2021
·
IF 4.311
Zhongliang Huang,Yujia Yuan,Miaomiao Song,Zhimian Hao,Jingran Xiao,Dongren Cai,Abdul-Rauf Ibrahim,Guowu Zhan
Herein, we fabricated a series of bimetallic Pt-Ni catalysts supported on mesoporous silica nanorods ( m SNR, specific BET surface area of 1802 m 2 g −1 ) to study the effect of Ni/Pt ratio on the product selectivity in CO 2 hydrogenation. Both monometallic Pt/ m SNR and Ni 50 Pt 50 / m SNR catalysts revealed negligible methane selectivity. However, methane became the major product only when increasing the Ni/Pt ratio up to 9. X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma (ICP) characterizations showed that the Pt/Ni ratio on the catalyst surface was appreciably higher than the bulk composition, suggesting the enrichment of Pt on the surface ( e.g. , Pt/Ni of 61/39 for Ni 50 Pt 50 / m SNR catalyst). The Pt/Ni ratio was crucial in determining the CH 4 /CO selectivity, and the addition of a tiny amount of Pt could improve the catalytic performance and stability of Ni/ m SNR. Among the different catalysts, Ni 98 Pt 2 / m SNR showed the best CO 2 conversion (59%) and CH 4 selectivity (96%) at 400 °C, 0.1 MPa, 9600 mL h −1 g cat −1 , and H 2 /CO 2 of 3. In-situ DRIFTS and temperature-programmed surface experiments suggested that the dissociated adsorption of CO 2 on the Pt site led to CO*, but the strongly adsorbed CO* cannot be further hydrogenated to CH 4 over the Pt site. In contrast, CO* could be further hydrogenated into CH 4 via CH x O* intermediates on adjacent Ni sites.
研究领域:
催化
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2024
·Vol. 53
·期 7
·2957-2963
·
IF 3.5
Peng Zhang,Sai Ma,Yujuan Zhang,Chaohui He,Tuoping Hu
The energy-saving separation of CO2/N2 and CH4/N2 in the energy industry facilitates the reduction of greenhouse gas emissions and replenishes energy resources, but is a challenging separation process. The trade-off between adsorption capacity and selectivity of the adsorbents is one of the key bottlenecks in adsorption separation technologies’ large-scale application in the above separation task. Herein, we introduced a series of fluoroborate or fluorosilicate salts (Cu(BF4)2, Zn(BF4)2 and ZnSiF6) into the open coordination nitrogen sites of aluminum-based metal–organic frameworks (MOF-253) to create multiple binding sites to simultaneously enhance the adsorption capacity and selectivity for the target gas. By the synergistic adsorption effect of metal ions (Cu2+ or Zn2+) and fluorinated anions (BF4− or (SiF6)2−), the single-component adsorption capacity and selectivity of salt-modified MOF-253 (MOF-253@Cu(BF4)2, MOF-253@Zn(BF4)2 and MOF-253@ZnSiF6) for CO2 and CH4 were effectively improved when compared to pristine MOF-253 at 298 K and 1 bar. In addition, the salt-modified MOF-253 has a moderate adsorption heat (<30 kJ mol−1) which could be rapidly regenerated at low energy by evacuation desorption. As confirmed by the ambient breakthrough experiments of MOF-253 and MOF-253@ZnSiF6, the real separation performance for both CO2/N2 (1/4) and CH4/N2 (1/4) was obviously improved. This work provides a feasible post-modification strategy on uncoordinated sites of the framework to improve adsorption separation performance and promote the development of ideal adsorbents with a view to realizing their application in the energy industry.
研究领域:
化学工程
·
材料科学
·
环境科学
·
能源工业
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Surfaces and Interfaces
·
2025
·
IF 6.3
Ming Liu,Nan Sun,Ruohan Xu,Tallat Munir,Shiyang Bai,Jihong Sun
The surfactant involvement in hydrothermal synthesis system of clinoptilolite (CP) is an effective strategy for regulating self-assemble of the aluminosilicate species. Herein, using cetyltrimethylammonium bromide (CTAB) as surfactant, the CTAB-assisted influences on nucleation behavior of CP were demonstrated via various characterizations. Especially, small angle X-ray scattering patterns were used to investigate the fractal structural evolutions of aluminosilicate species in their sol-gel phase. The results indicated that the primary building structural units with 8- and 10-membered rings appeared in the early induced stage gradually aggregated into the worm-liked particles with the prolonged crystallization time. Among them, the nucleation process was initiated by reorganization via the solution-mediated transport and thereafter appeared the pseudo-layered structures with the core (aluminosilicate species)-shell (CTAB) features at the liquid-solid interfaces. The irregulated lamellas with the heulandite structures increased in size of around 70 nm until reaching the maximum of 90 nm, then followed the occurrences of the re-dissolving and repaid growth. Especially, the lamellar nuclei growth showed the transformations from loose mass fractals to dense surface fractals with the extensions of the induced time. In which, the interfacial solvation layer thickness increased from 1.04 to 2.87 nm for CTAB-assisted CP, thicker than that (0.63–2.08 nm) for pure-CP. These demonstrations suggested that the additive CTAB in the induced stage inhibited the agglomeration of the aluminosilicate species and following growth of the crystal nuclei via the solvated attachments pathway. Finally, using the irregulated particle as an adsorbent, the CO 2 adsorption and CO 2 /CH 4 selectivity were preliminarily explored.
研究领域:
材料科学
·
化学工程
·
物理化学
·
纳米技术
·
吸附科学
·
矿物学
✓ 已验证
产品关联
DOI
高影响因子