SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xuebi Du,Shichao Feng,Jianquan Luo,Yongbing Zhuang,Weijie Song,Xuewei Li,Yinhua Wan
Amine-functionalized and metal doped metal–organic frameworks (MOFs) will enable further enhancement of CO 2 adsorption, which holds great promise in mixed matrix membranes (MMMs) for CO 2 /N 2 separation. Four kinds of UiO66 with different sizes have been successfully fabricated by introduction of Ce and/or amino groups in UiO66. The influence of Ce doping on the UiO66 is greatly related to the ligand. Compared with ZrUiO66, the CeZrUiO66 has bigger particle size, lower BET specific surface area and pore volume and a worse CO 2 adsorption capacity. Interestingly, the tendency of Ce-doped ZrUiO66-NH 2 is contrary to the aforementioned. In particular, bimetallic CeZrUiO66-NH 2 has an ultramicroporous structure, small particle size, rich crystal defect, superb CO 2 capture capacity and high CO 2 /N 2 adsorption selectivity, suggesting that the simultaneous introduction of Ce and amino groups is conducive to the enhancement of CO 2 separation. The intrinsic ultramicroporous structure of CeZrUiO66-NH 2 not only offers fast and low resistance transport channels for CO 2 , but also supplies more sites for CO 2 adsorption owning to the doping of Ce and the amino groups. As a result, Pebax/CeZrUiO66-NH 2 (3 wt%) MMMs show the CO 2 permeability of 100.7 Barrer and the CO 2 /N 2 ideal selectivity of 76.4, which is close to Robeson upper bound from 2008. Meanwhile, the Pebax/CeZrUiO66-NH 2 (3 wt%) MMMs present relatively good pressure resistance, which would be advantageous in terms of industrial application.
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CATALYSIS LETTERS
·
2023
·
IF 2.8
Chen Yiming,Hou Zhanggui,Wang Chuan,Ma Xin,Yang Hong,Wang Wen,Zhou Ling,Zhang Yi
As well known, the industrial methanation process needs highly active and stable catalysts obtained from cheap and abundant elements. In this work, we propose a high-loaded Ni/Al 2 O 3 catalyst promoted by manganese. Among them, the 20Ni2Mn/Al 2 O 3 catalyst exhibits the best CO 2 conversion (90.5%) and excellent methanation stability at 250 °C. In addition, the roles of the Mn promoter on CO 2 conversion and selectivity were investigated in detail. The features of natural and promoted catalysts are described through XRD, XRF, BET, TEM, H 2 -TPR, CO 2 -TPD, and operando DRIFTS techniques. Based on various characterization results, the addition of Mn will greatly reduce the Ni particle size and improve the Ni dispersion on the alumina support. Furthermore, compared to the unpromoted catalyst, Mn promoted catalysts show better reducibility and have more medium basic sites. And these medium basic sites are favorable to the adsorption and activation of CO 2 . In-situ DRIFTS experiments for CO 2 methanation reveal that manganese could promote the monodentate carbonate hydrogenated to formate rapidly, which could be faster converted towards CH 4 , contributing to significantly improved activity of the Mn promoted Ni/Al 2 O 3 catalyst. Graphical Abstract
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RSC Advances
·
2023
·Vol. 13
·期 25
·17362-17369
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IF 3.9
Zhe Zhang,Fanhao Kong,Bizhen Yuan,Yinnian Liao,Xiue Ren,Yu Hou
Solar-driven CO2 reduction into fuels and sustainable energy has attracted increasing attention around the world. However, the photoreduction efficiency remains low due to the low efficiency of separation of electron–hole pairs and high thermal stability of CO2. In this work, we prepared a CdO decorated CdS nanorod for visible light driven CO2 reduction. The introduction of CdO facilitates the photoinduced charge carrier separation and transfer and acts as an active site for adsorption and activation of CO2 molecules. Compared with pristine CdS, CdO/CdS exhibits a nearly 5-fold higher CO generation rate (1.26 mmol g−1 h−1). In situ FT-IR experiments indicated that CO2 reduction on CdO/CdS may follow a COOH* pathway. This study reports the pivotal effect of CdO on photogenerated carrier transfer in photocatalysis and on CO2 adsorption, which provides a facile way to enhance photocatalytic efficiency.
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PubMed
高影响因子
Small
·
2023
·Vol. 19
·期 39
·2302530
·
IF 13.3
Xiaotong Li,Minkai Qin,Xiuju Wu,Xiangzhou Lv,Jianghao Wang,Yong Wang,Hao Bin Wu
Electrochemical CO 2 reduction reaction (CO 2 RR) is a promising strategy for waste CO 2 utilization and intermittent electricity storage. Herein, it is reported that bimetallic Cu/Pd catalysts with enhanced *CO affinity show a promoted CO 2 RR performance for multi-carbon (C2+) production under industry-relevant high current density. Especially, bimetallic Cu/Pd-1% catalyst shows an outstanding CO 2 -to-C2+ conversion with 66.2% in Faradaic efficiency (FE) and 463.2 mA cm −2 in partial current density. An increment in the FE ratios of C2+ products to CO for Cu/Pd-1% catalyst further illuminates a preferable C2+ production. In situ Raman spectra reveal that the atop-bounded CO is dominated by low-frequency band CO on Cu/Pd-1% that leads to C2+ products on bimetallic catalysts, in contrast to the majority of high-frequency band CO on Cu that favors the formation of CO. Density function theory calculation confirms that bimetallic Cu/Pd catalyst enhances the *CO adsorption and reduces the Gibbs free energy of the C C coupling process, thereby favoring the formation of C2+ products.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yuhang Yang,Chuanwen Zhao,Pengxin Zeng,Yuhao Wang,Xue Qin,Yueyue Gao,Yafei Guo,Ruilin Wang,Jian Sun
Suitable molding and granulation methods are crucial, and an outstanding sphere structure can play a better role in the future scale-up industrial application of K 2 CO 3 -based CO 2 adsorbent. Water will form a large contact angle on the surface of hydrophobic solution and become sphericity water. In this work, hydrophobic powders (polyethylene (PE), TiO 2 , and SiO 2 ) were selected in the hydrophobic interface-assisted method. The CO 2 adsorption capacity of TiO 2 pellets is 0.50 mmol/g, while that of PE pellets is 0.24 mmol/g, and finally that of SiO 2 pellets is 0.36 mmol/g. Then, experiment proved that high temperature (>500 ℃) makes the hydrophobic powders (i.e, TiO 2 and SiO 2 ) lose hydrophobicity which make water molecules diffuse faster, while PE is completely decomposed at high temperature. Compared with the pellets calcined at 300 ℃, the TiO2 pellets calcinated at 500 ℃ have an adsorption capacity of 0.70 mmol/g, which is over 1.72 times that of the original pellets, and the other two hydrophobic surfaces are also improved to some extent. Additionally, the appropriate ratio of low-temperature pore forming agent (i.e., urea) can help improve the adsorption performance, while excessive addition will lead to poor CO 2 adsorption performance. In addition, the K 2 CO 3 /Al 2 O 3 pellets also exhibited desirable mechanical properties, with an optimal compressive strength of 41 Mpa. Therefore, the loss of hydrophobicity leads to more active diffusion of water molecules, which may provide a new idea for the future development of CO 2 adsorbents and other areas.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 15
·8248-8255
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IF 11.9
Liang Shen,Wenhao Zhang,Yifei Feng,Jing Xu,Minghui Zhu
Hydrogenation of CO2 to produce high-value chemicals is a response to increasing environmental and energy concerns. The target products of CO2 hydrogenation, methane and CO, are both important energy sources and raw materials for the production of higher hydrocarbons. Therefore, it is very important to understand the mechanism of selectivity control of catalysts. In this work, we aim to elucidate the selectivity regulation of Zn on Ni catalysts, which has been extensively studied in the literature without reaching a consensus. We have prepared a series of catalysts with different Zn content and systematically investigated the relationship between their structural evolution and selectivity. It is found that the introduction of Zn preferentially forms an alloy with Ni and at higher loadings is present as ZnOx, which participates in the strong metal–support interaction (SMSI). The conversion of the active sites into a Ni–Zn alloy hinders further hydrogenation of the adsorbed CO intermediates and makes the catalyst CO-selective. The presence of the Ni–ZnOx interface changes the CO2 activation mechanism from an association pathway to a redox pathway.
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Nano Energy
·
2023
·
IF 17.6
Jiaqi Zhao,Zhenhua Li,Pu Wang,Peng Miao,Run Shi,Geoffrey I.N. Waterhouse,Tierui Zhang
CO photo-hydrogenation is currently attracting a lot of interest as a low energy input technology for the sustainable production of olefins . Herein, a novel photo-driven Fischer-Tropsch to olefins (FTO) catalyst was synthesized by physical mixing a layered-double-hydroxide-derived cobalt catalyst (LD-Co) with a hydrophobic polydivinylbenzene (PDVB). The obtained LD-Co/PDVB catalyst synergistically harnessed the photothermal and catalytic properties of LD-Co with the hydrophobic properties of PDVB to deliver outstanding photothermal FTO performance. Under ultraviolet-visible irradiation, hydrophobic LD-Co/PDVB delivered a higher CO photo-hydrogenation activity than hydrophilic LD-Co, together with a high olefin selectivity (42.72%−50.49%) and greatly suppressed CO 2 selectivity (2.89%−11.50%) compared to LD-Co (12.65%−30.61%) at 180–195 °C. Water vapor adsorption-desorption experiments and water-gas shift (WGS) reaction tests revealed that the hydrophobic modification acted to suppress the WGS reaction, thereby boosting the olefin production and suppressing CO 2 selectivity. The findings demonstrated that a simple hydrophobic modification can be used to regulate the activity and selectivity of catalysts for photothermal FTO reactions, opening new vistas towards improved photo-driven olefin production.
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Tong Dou,Jinqing He,Shuteng Diao,Yiping Wang,Xuhui Zhao,Fazhi Zhang,Xiaodong Lei
As the “emission peak and carbon neutrality peak” are proceeding all over the world, CO 2 electroreduction is studied extensively as it is a powerful way to transform CO 2 into value-added products. The earth-abundant Sn-based materials and copper sulfides as electrochemical catalysts have shown activity for generating formate from CO 2 electroreduction. Herein, the composite of CuS and S-doped SnO 2 (CuS/SnO 2 -S) was synthesized by a redox reaction under room temperature. The unique structural reconstruction of CuS/SnO 2 -S nanoparticles to Cu/Sn/Cu 6.26 Sn 5 nanowires decreases the energy barrier of the adsorption of CO 2 , and increases the adsorption of *H, primarily suppressing the competing reaction of hydrogen evolution reaction (HER). As a result, at − 0.8 V vs. RHE , it reaches an electrochemical CO 2 -to-formate conversion with a Faradaic efficiency (FE) of 84.9% at a yield of 8860 µmol h −1 cm − 2 under a partial current density of ∼18.8 mA cm − 2 in an H-type reactor. This study provides significant insight into the structural evolution of the CuSn sulfides and the mechanism of formate formation.
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Green Energy & Environment
·
2023
·
IF 13.3
Liu Han,Cheng-wei Wang,Shan-shan Luo,Ying-tang Zhou,Bing Li,Ming Liu
Employing crystal facets to regulate the catalytic properties in electrocatalytic carbon dioxide reduction reaction (eCO 2 RR) has been well demonstrated on electrocatalysts containing single metals but rarely explored for bimetallic systems. Here, we synthesize ZnSn(OH) 6 (ZSO) microcrystals (MCs) with distinct facets and investigate the facet effects in eCO 2 RR. Electrochemical studies and in situ Fourier Transform Infrared Spectroscopy (in situ-FTIR) reveal that ZSO MCs produce mainly C1 products of HCOOH and CO. The {111} facet of the ZSO MCS exhibits higher selectivity and faradaic efficiency (FE) than that of the {100} facet over a wide range of potentials (−0.9 V ∼ −1.3 V versus RHE). Density Functional Theory (DFT) calculations elucidate that the {111} facet is favorable to the adsorption/activation of CO 2 molecules, the formation of intermediate in the rate-determining step, and the desorption of C1 products of CO and HCOOH molecules.
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Journal of Energy Chemistry
·
2019
·
IF 5.162
Jie Du,Wen-Cui Li,Zhan-Xin Ren,Li-Ping Guo,An-Hui Lu
Porous carbon materials with developed porosity, high surface area and good thermal- and chemical-resistance are advantageous for gas adsorption and separation. However, most carbon adsorbents are in powder form which exhibit high pressure drop when deployed in practical separation bed. While monolithic carbons have largely addressed the pulverization problem and preserved kinetics and usually suffer from abrasion during multiple adsorption-desorption cycles. Herein, we proposed the designed synthesis of mechanically robust carbon monoliths with hierarchical pores, solid nitrogen-containing framework. The synthesis started with the polymerization of resorcinol and formaldehyde under weakly acidic conditions generated from cyanuric acid, and then an appropriate amount of hexamethylenetetramine (HMTA) was added as a crosslinker to prompt the formation of three dimensional frameworks. After carbonization process, the as-obtained porous carbon monoliths have a high radial compressive strength of 886 N/cm as well as a BET specific surface area of up to 683 m 2 /g. At approximately 1 bar, the CO 2 equilibrium capacities of the monoliths are in the range of 3.1–4.0 mmol/g at 273 K and of 2.3–3.0 mmol/g at 298 K, exhibiting high selectivity for the capture of CO 2 over N 2 from a stream which consists of 16.7% (v%) CO 2 in N 2 . Meanwhile, they undergo a facile CO 2 release in an argon stream at 298 K, indicating a good regeneration capacity. After cycle testing, sieving and regeneration, the adsorbent has no mass loss, compared to that of its fresh counterpart.
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ELECTROCHIMICA ACTA
·
2019
·
IF 5.383
Yuning Zhang,Lin Liu,Lei Shi,Tingting Yang,Dongfang Niu,Shuozhen Hu,Xinsheng Zhang
The effects of halide ions (F − , Cl − , Br − , and I − ) on nanoporous Ag electrode for reduction of CO 2 to CO were systematically assessed. The electrochemical measurements indicate that the catalytic performance of nanoporous Ag is closely related to the affinity of halide ions to Ag. The current density and Faradaic efficiency for CO production simultaneously increase with the increase of the radius of halide ions from F − to Cl − and then to Br − , and the disparity between catalytic performance will further widen with the negative shift of potential. While the nanoporous Ag in the presence of I − first exhibits the poorest electrocatalytic performance at low potential (<−0.69 V vs . RHE), then reverses the situation at high potential (>−0.89 V vs . RHE) in comparison to the other halide ions. Tafel plots indicate that the adsorption of halide ions on the surface of nanoporous Ag influences mechanistic pathways for CO 2 reduction reaction. 8 h durability test demonstrates that the nanoporous Ag is catalytically stable in a mixed electrolyte containing bromide with only less than 5% deactivation. The density functional theory calculations enlighten that the weakened interaction between Ag atoms on the surface of electrocatalyst in the presence of halides can significantly enhance the binding energy of the intermediate COOH*, and thus effectively lowers the overpotential of CO 2 reduction reaction.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Shiyu Bie,Meili Du,Wenxiang He,Huigang Zhang,Zhentao Yu,Jianguo Liu,Meng Liu,Wuwei Yan,Liang Zhou,Zhigang Zou
Efficient electrocatalysts for Li2CO3 decomposition play an important role in Li–CO2 batteries. In this paper, carbon nanotubes (CNTs) decorated with RuO2 is firstly introduced as cathode materials for Li–CO2 batteries. The CNT@RuO2 composite can not only deliver a high specific capacity but also a lower charge voltage. With the CNT@RuO2 cathodes, the Coulombic efficiency still remains around 100% until the 15th cycle. The charge voltage of early 30 cycles at a current of 50 mA·g–1 with a capacity limit of 500 mAh·g–1 can be fully lowered under 4.0 V. Particularly, the CNT@RuO2 cathode can realize most decomposition of prefilled Li2CO3 and show a platform at around 3.9 V. This catalytic activity toward both in situ formed and preloaded Li2CO3 is more feasible for practical application in complex environment.
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