JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Ying He,Zhuoyue Wang,Aihui Cao,Xiao Xu,Junqiang Li,Bo Zhang,Longtian Kang
The zinc-based photocatalysts for CO 2 reduction have attracted increasing attention, however, usually exhibit low CO 2 -to-CH 4 selectivity. Here, the graphene oxide (GO)-coated zinc tetraphenylporphyrin (ZnTPP/GO) nanocomposites are successfully synthesized through a simple method. It is found that with the increase of GO content, the crystallinity of ZnTPP nanocrystals enhances with the size decrease, and then the light absorption can easily match with the solar spectrum. The optimal ZnTPP/GO sample exhibits the CH 4 evolution rate of 41.6 μmol g −1 h −1 and CH 4 selectivity of >95%, which are higher than those of ZnTPP nanocrystals (7.8 μmol g −1 h −1 and 50.3%). The systematic characterizations confirm that the generation of axial coordinated Zn O C bonds between ZnTPP and GO plays a key role in the formation of ZnTPP/GO nanostructure and their synergic effect on photocatalytic CO 2 reduction. The encapsulation of GO on ZnTPP nanocrystals not only promotes the CO 2 adsorption, interfacial reaction, and stability, but also accelerates the separation of photoinduced carriers on ZnTPP (0.1 ps vs. 425.9 ps), the transportation from ZnTPP to GO (2.3 ps vs. 83.6 ps), and their final enrichment on GO. This work provides a new strategy to apply graphene and organic nanomaterials in artificial photosynthesis.
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高影响因子
AICHE JOURNAL
·
2022
·Vol. 68
·期 5
·e17589
·
IF 4.167
Jiaqi Liu,Xuan Tang,Xiaowu Liang,Luogang Wu,Feifei Zhang,Qi Shi,Jiangfeng Yang,Jinxiang Dong,Jinping Li
Various adsorbents for CH 4 /N 2 separation were developed to enrich low-concentration coal-mine methane. Most are hydrophilic and cannot treat moist coal-mine methane. We report for the first time a microporous zeolitic imidazolate framework Co(dcIm) 2 (TUT-100) with superhydrophobic properties for CH 4 /N 2 separation. The CH 4 adsorption capacity and CH 4 /N 2 selectivity were as high as 45.29 cm 3 /cm 3 and 6.3 (298 K, 1 bar), respectively, which results from the suitable SOD cage size (0.80 nm). The H 2 O adsorption was lower than 6.3 cm 3 /g at 298 K and near saturated pressure due to the hydrophobic group Cl. Breakthrough experiments were carried out to indicate the significant potential for CH 4 /N 2 adsorption separation in a humid environment. The adsorption behavior of the gas mixture on the TUT-100 was investigated by the Grand Canonical Monte Carlo method and coupled with the experimental data.
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ADVANCED MATERIALS
·
2022
·Vol. 34
·期 16
·2200756
·
IF 32.086
Xi Lin,Shuhui Xia,Liang Zhang,Yuanyuan Zhang,Songmei Sun,Yuehui Chen,Shuo Chen,Bin Ding,Jianyong Yu,Jianhua Yan
Achieving high selectivity and conversion efficiency simultaneously is a challenge for visible-light-driven photocatalytic CO 2 reduction into CH 4 . Here, a facile nanofiber synthesis method and a new defect control strategy at room-temperature are reported for the fabrication of flexible mesoporous black Nb 2 O 5 nanofiber catalysts that contain abundant oxygen-vacancies and unsaturated Nb dual-sites, which are efficient towards photocatalytic production of CH 4 . The oxygen-vacancy decreases the bandgap width of Nb 2 O 5 from 3.01–2.25 eV, which broadens the light-absorption range from ultraviolet to visible-light, and the dual sites in the mesopores can easily adsorb CO 2 , so that the intermediate product of CO* can be spontaneously changed into *CHO. The formation of a highly stable Nb CHO* intermediate at the dual sites is proposed to be the key feature determining selectivity. The preliminary results show that without using sacrificial agents and photosensitizers, the nanofiber catalyst achieves 64.8% selectivity for CH 4 production with a high evolution rate of 19.5 µmol g −1 h −1 under visible-light. Furthermore, the flexible catalyst film can be directly used in devices, showing appealing and broadly commercial applications.
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Journal of CO2 Utilization
·
2022
·
IF 8.321
Nicui Yuan,Yuxin Mei,Yuwei Liu,Yating Xie,Baining Lin,Yonghua Zhou
The development of efficient and highly selective photocatalysts is a key point for the photocatalytic conversion of CO 2 . In this paper, a composite catalyst UiO-66-NH 2 /Ce(HCOO) 3 (simplified to UNH/Ce(HCOO) 3 ) was fabricated by one pot method with CeCO 3 OH as the precursor. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) characterizations results confirmed that UNH was dispersed on the surface of Ce(HCOO) 3 and strongly interacted with it via Ce-N bond. The yield of CH 4 on the optimal UNH/Ce(HCOO) 3 catalyst reached 3 times of that on pristine UNH, up to 128.81 μmol g −1 , with the CH 4 selectivity of 71.9 %, and the R electron reached 286.46 μmol g −1 h −1 . The UV–vis diffuse reflection spectra and photoelectrochemical tests results confirmed that the improved photocatalytic CO 2 reduction performance and high CH 4 selectivity could be attributed to the formation of the type-Ⅱheterojunction of UNH/Ce(HCOO) 3 with abundant Ce 3+ , which expanded the visible light absorption range, accelerated the separation and transfer rates of photogenerated charges, and thus efficiently promoted the multi-electron reduction reaction of CO 2 to CH 4 . In addition, the reaction temperature affected profoundly the cycle performance of the catalyst. The results presented here illustrated the possibility for improving the stability of UNH/Ce(HCOO) 3 -1.80 by decreasing reaction temperature.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Ke Wang,Xianhe Li,Nan Wang,Quanhao Shen,Maochang Liu,Jiancheng Zhou,Naixu Li
Solar photocatalysis has long relied on the rational design of semiconductor photocatalysts. Herein, a ternary meso-TiO2@ZnIn2S4/Ti3C2 MXene photocatalyst is prepared and demonstrated with a core–shell structure accompanied by few-layered Ti3C2 Mxene on the ZnIn2S4 shell. The success of the synthesis depends on a two-step method consisting of hydrothermal and electrostatic self-assembly procedures. The ternary heterojunction exhibits a good behavior for photocatalytic CO2 reduction. A mechanism study of the photocatalytic reaction indicates that the photogenerated charges transfer in a Z-scheme pathway. Moreover, the construction of the Schottky junction between metallic Ti3C2 and TiO2@ZnIn2S4 is extremely effective for the reduction reaction. Consequently, the photocatalytic rates toward CO and CH4 production are up to 30.5 and 34.0 μmol/g within 3 h of illumination by simulated sunlight, respectively, while the CH4 selectivity reaches 52.7%. This work provides a good strategy to achieve highly efficient photocatalytic CO2 reduction.
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AICHE JOURNAL
·
2020
·Vol. 66
·期 6
·e16936
·
IF 3.519
Xiaomin Zhang,Wenjie Xiong,Lingling Peng,Youting Wu,Xingbang Hu
Recently, the selective removal of H 2 S and CO 2 has been highly desired in natural gas sweetening. Herein, four novel azole-based protic ionic liquids (PILs) were designed and prepared through one-step neutralization reaction. The solubility of H 2 S (0–1.0 bar), CO 2 (0–1.0 bar), and CH 4 (0–5.0 bar) was systematically measured at temperatures from 298.2 to 333.2 K. NMR and theoretical calculation were used to investigate the reaction mechanism between these PILs and H 2 S. Reaction equilibrium thermodynamic model (RETM) was screened to correlate the H 2 S solubility. Impressively, 1,5-diazabicyclo[4,3,0] non-5-ene 1,2,4-1H-imidazolide ([DBNH][1,2,4-triaz]) shows the highest H 2 S solubility (1.4 mol/mol or 7.3 mol/kg at 298.2 K and 1.0 bar) and superior H 2 S/CH 4 (831) and CO 2 /CH 4 (199) selectivities compared with literature results. Considering the excellent absorption capacity of H 2 S, high H 2 S/CH 4 , and CO 2 /CH 4 selectivity, acceptable reversibility, as well as facile preparation process, it is believed that azole-based PILs provide an attractive alternative in natural gas upgrading process.
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ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Chunyu Li,Chao Wu,Baoquan Zhang
Blending porous inorganic fillers into polymers to fabricate mixed matrix membranes (MMMs) is an efficient method to acquire good-quality membranes for CO2 separation and purification. The poor interface coupling between bulky filling particles and polymer phase in MMMs results in reduced mechanical strengths with low separation performances. The novel two-dimensional (2D) and ultrathin α-Ni(im)2 nanosheets with high aspect ratios are herein synthesized and blended with Pebax MH 1657 to prepare MMMs. The larger contacting area and strong hydrogen bonding between α-Ni(im)2 nanosheets and Pebax improve their compatibility to form defect-free MMMs. The ultrathin α-Ni(im)2 nanosheets in MMMs can effectively enhance CO2/CH4 selectivity based on molecular sieving. With the addition of 2 wt % of α-Ni(im)2 nanosheets, the as-prepared MMMs exhibit CO2/CH4 selectivity up to 33.4 with a permeability of 100.6 Barrer. Compared with pure Pebax membrane, the separation selectivity shows a 72% increase with no significant change in CO2 permeability.
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ADVANCED ENGINEERING MATERIALS
·
2023
·Vol. 25
·期 22
·2301062
·
IF 3.6
Binxia Yuan,Hong Qian,Lan Cao,Rui Zhu,Weiling Luan
Herein, H + in oxalic acid is used instead of Na + to obtain titanate nanosheets through P200 hydrolysis, which further curls to form a multilayer TiO 2 nanotubes (NTs) structure. Then, Cu 2 O quantum dots (QDs) are successfully loaded on TiO 2 NTs via a hydrothermal method using fructose as a reducing agent. The optical, impedance, and photocurrent tests indicate that the composite structure improves its optoelectronic performance. The photocatalytic H 2 production and CO 2 reduction efficiency of Cu 2 O QDs/TiO 2 NTs are lower than those of TiO 2 NTs. However, the molar ratio of CH 4 to CO produced by CO 2 reduction of Cu 2 O QDs/TiO 2 NTs composite catalyst is greater than that of pure TiO 2 NTs. The CH 4 production accounts for 97%, indicating that the composite catalyst has a high CH 4 selectivity. The experimental and density functional theory calculation results prove that the Z-scheme heterojunction accelerates the separation and transfer of photogenerated carriers, and broadens the absorption range of visible light.
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CARBOHYDRATE POLYMERS
·
2023
·
IF 11.2
Wenkai Zhu,Meiling Chen,Jieun Jang,Minsu Han,Yeonggyun Moon,Junghwan Kim,Jungmok You,Song Li,Teahoon Park,Jeonghun Kim
Nanocellulose-based aerogels have been considered as one of the ideal candidates for CO 2 capture in practical applications owing to their lightweight and porous properties. Additionally, various adsorbents with amine groups have been widely used as effective CO 2 capture and storage strategies. Herein, amino-functionalized aerogels were prepared by sol-gel and freeze-drying methods using two typical nanocelluloses (cellulose nanofibrils (CNFs) and cellulose nanocrystals (CNCs)) as substrates. In addition, the reaction parameters for grafting and amino functionalization were optimized. The CNC and CNF aerogels could be easily modified by the hydrothermal growth of the amino group, and they exhibited attractive properties in terms of CO 2 adsorption, recyclability, thermal stability , hydrophobicity , and CO 2 /CH 4 mixture separation. The amino-functionalized CNF aerogel exhibited superior performance to the CNC aerogel, which was attributed to the increased cross-linking binding sites for hydrogen bonding in the CNF aerogel. The results of this study indicated that amino-functionalized nanocellulose aerogels can be considered a promising biodegradable, sustainable, and environmentally friendly material for CO 2 capture and removal of CO 2 from CH 4 .
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 27
·70884-70896
·
IF 5.8
Li Ke,Zhu Yuqiu,Wang Zixuan,Chen Dingkai,Wu Wenwei,Luo Yongming,He Dedong
High concentration of H 2 S in acidic natural gas will lead to poisoning of catalysts for hydrogen production by methane steam reforming, thus limiting the further use of natural gas. Reforming CH 4 by H 2 S can be considered as an alternative route to hydrogen production from methane. This process not only achieves the removal of H 2 S but also obtains chemical raw material CS 2 and clean energy H 2 . By impregnating the Mo source on SiO 2 treated with hydrogen peroxide and then using the catalyst in the CH 4 /H 2 S reforming reaction, we surprisingly found that the conversion rate of CH 4 and H 2 S increased from 28 and 32% to 34% and 43%, respectively, after hydrogen peroxide treatment. The H 2 production rate and the yield of CS 2 increased from 20 mmolH 2 /(g Mo *min) and 52% to 30 mmolH 2 /(g Mo *min) and 65%, respectively. Combining with characterization methods such as X-ray diffraction (XRD), hydrogen temperature programmed reduction (H 2 -TPR), 1 H-based solid-state nuclear magnetic resonance ( 1 H MAS NMR), X-ray photoelectron spectroscopy (XPS), Raman spectra (RS), and transmission electron microscopy (TEM), we found that the hydroxyl concentration of the support increased after hydrogen peroxide treatment, which led to the strengthening of the force between the metal and the support, which was easy to form low-level and small-size MoS 2 , exposing more active sites, and further improving the catalytic activity. This method provides a new idea for hydrogen production by CH 4 /H 2 S reforming and the development of high-performance MoS 2 -based catalysts.
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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.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Zhihao Zhou,Soomro Sarmad,Chao Huang,Guoshu Deng,Zhenkun Sun,Lunbo Duan
Ni-based catalysts supported on ordered mesoporous Al 2 O 3 with 2-D hexagonal and 3-D cubic pore structures are synthesized via evaporation-induced self-assembly for catalyzing dry CH 4 reforming to produce syngas . The Ni–Al 2 O 3 catalysts with 3-D pore structure exhibit higher activity in terms of CH 4 and CO 2 conversions than those with 2-D pore symmetry, due to the better mass transfer of the 3-D interconnected pore structure for the accessibility of Ni 0 active sites. And a higher Ni content slightly promotes catalytic activity , owing to more exposed active sites. However, a higher Ni content causes more severe carbon deposition during long-term reaction. During the long-term stability tests, the catalysts with 2.5 wt% Ni maintain the highest stability regardless of the pore structure, and the catalyst with 3-D pore structure is more advantageous to both activity and stability. Meanwhile, the catalyst with 2.5 wt% Ni and 3-D pore structure shows the lowest carbon deposition.
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