COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
·
IF 5.2
Qiang Wang,Yaru Li,Zichen Yu,Xuewen Li,Shouhua Yin,Wen Ji,Yonghua Hu,Weiping Cai,Xianbiao Wang
Highly porous carbon adsorbent is much desired to diminish greenhouse effect caused by CO 2 emission and benefit for subsequent carbon cycle . Herein, a low-cost and environment-friendly carbonization strategy was reported for preparation of highly porous carbon derived from biomass. Such carbonization is a synergistic process with hydrothermal treatment coupled with a subsequent pyrolysis using sugarcane as biomass. The obtained hydrothermal-pyrolysis derived porous carbon (HPC) has a BET surface area of 938 m 2 /g, which is much higher than that of carbon produced through direct pyrolysis (PC, 528 m 2 /g). During the hydrothermal carbonization pretreatment, highly thermostable aromatic skeletons are formed and converted to carbon skeletons in the post-pyrolysis process, leading to formation of highly stable micropores and higher surface area. Further, HPC shows remarkable adsorption ability of CO 2 (2.8 mmol/g, 25 °C, 1 bar), higher than that of PC (2.1 mmol/g). In addition, the HPC exhibits high CO 2 /N 2 adsorption selectivity and recyclability, demonstrating its potential application in CO 2 capture. This work not only gives new light for tailoring carbon materials with highly porous structure but also provides novel adsorbent for CO 2 adsorption.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 20
·9842-9851
·
IF 3.3
Li Luo,Jie Deng,Yingying Wang,Qiang Tang,Mengyue Hou,Ziyue Zhang,Shijian Lu,Yongdong Chen
Developing efficient catalysts is crucial for the chemical utilization of CO2, which would be conducive to solving both environmental issues and the resource crisis. In this work, a basalt fiber (BF)-supported CuNi catalyst was constructed for the conversion of CO2 and methanol to dimethyl carbonate (DMC). In order to optimize the surface properties of BF, the pristine BF (BF-U) was modified by HCl (BF-H) and NaOH (BF-N) solutions. The influence of the BF surface properties on the physicochemical state of CuNi and the catalytic performance of the supported CuNi/BF catalysts was systematically investigated. The results showed that the CuNi/BF-N monolithic catalyst had the best activity, and the yield of DMC reached 12.9%. SEM, XRD, and XPS characterizations exhibited that the CuNi nanoalloy particles were uniformly distributed on BF-N and possessed high Cu0/1+ and Ni0 contents. This contributed to the abundant CO2 adsorption sites, as evidenced by CO2-TPD, especially for the medium-strength CO2 adsorption sites, which was responsible for the superior catalytic activity. This study provides an efficient catalyst for the synthesis of DMC from CO2 and methanol and can serve as a reference for industrial catalyst design.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Wei Bi,Ling Zhang,Hao Jiang,Chunzhong Li,Yanjie Hu
The precise regulation of the nano-catalyst structure is a big challenge that limits the application of photocatalytic technology in CO 2 reduction. Herein, to improve the utilization of sunlight, the separation and transfer efficiency of photogenerated electron-hole pairs, and the surface catalytic reaction process, CuInS 2 /C/TiO 2 (CIS/C/T) hierarchical tandem heterostructure have been rationally designed. Multiple in-situ characterizations and DFT simulations show that CQDs not only act as a co-catalyst, but also act as a bridge between TiO 2 (T) and CuInS 2 (CIS), which further attribute to the efficient separation and enrichment of photogenerated electron-hole pairs while effectively avoiding the recombination. In consideration of the excellent broad-spectrum absorption, the CO 2 -to-CO photoreduction performance of the optimal CIS/C/T reaches up to 7.73 μmol g -1 h −1 , about 3.16 times enhancement of C/T. Combined with in-situ DRIFTs, the intrinsic structure–activity relationship is pointed out, and extended to other similar TiO 2 -based catalytic systems (In 2 S 3 /C/TiO 2 ). This work will provide a new universal strategy for the design and synthesis of high-performance nano-photocatalysts.
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TALANTA
·
2021
·
IF 6.057
Lijun Xu,Dongguo Xue,Jialin Sai,Lu Zhou,Renjun Pei,Aihua Liu
Although enzyme mimics have been widely developed, limited catalytic efficiency is still a bottleneck, especially under neutral condition. Herein, we reported the bioactive quinaldic acid (QA) significantly boosted the peroxidase-like activity of Co 2+ in the presence of bicarbonate (HCO 3 − ). With 2,2′-azino-bis-(3-ethylbenzothiazoline-6-sulphonate) (ABTS) as the substrate, the catalytic activity of Co 2+ (1 μM) was increased by over 300 times upon adding 100 μM QA. The formed Co 2+ complex had much higher turnover number (5.52 min −1 ) than that of cobalt-based nanozymes (0.011–0.51 min −1 ) in decomposing H 2 O 2 . Based on this system, ultrasensitive colorimetric methods for the detection of Co 2+ , bicarbonate and urease activity were achieved with limits of detection of 4.6 nM, 40 μM and 0.00125 U/mL, respectively. For the first time, this work established an ultrasensitive method for the detection of urease activity by activating a peroxidase-like mimic with the produced HCO 3 − .
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PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
·
IF 4.539
Lisha Sheng,Jie Lei,Zhenqian Chen,Yi Wang
Type I porous liquids (PLs) containing porosity are promising candidates for gas sorption and separation, homogeneous catalysis , and so forth. In this research, large porous silica nanoparticles (PSNs) and hollow wormhole silica nanoparticles (HSNs) are reported to fabricate Type I PLs through a facile synthetic strategy, where polyether amine is linked to nanoparticles by the silane coupling agent for CO 2 capture. Experimental results showed that canopies endow PSNs and HSNs with excellent fluidity along with the thermal stability of PLs at high temperature. The CO 2 sorption capability and dispersion stability were profoundly influenced by the specific surface area and pore size of PLs cores. At 25 °C and 2 bar, the CO 2 sorption capacities of pure M2070, PL_1_M2070, PL_2_M2070, and PL_3_M2070 were 10.9317 cm 3 /g, 9.1295 cm 3 /g, 6.2504 cm 3 /g, and 5.3518 cm 3 /g, respectively. Results showed that CO 2 sorption capability of porous silica nanoparticle assisted PLs with a large specific surface area and small pore sizes was superior. If the pore size was large enough, canopy would enter and fill the pores of silica nanoparticles, preventing part pores and polyether amine from offering active CO 2 sorption sites, thereby minimizing the CO 2 sorption and affecting the stability of the PLs. Sorption kinetics fitting results showed that the CO 2 sorption of PLs was the combination of physical dissolution and chemisorption . Furthermore, the adsorption capacity of PL_1_M2070 was 90.5% of the original CO 2 adsorption capacity after 10 adsorption/desorption cycles, indicating excellent recyclability.
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Membranes
·
2021
·Vol. 12
·期 1
·8
·
IF 4.106
Yunzhao Guo,Wenbo Qi,Kaiyun Fu,Xianfu Chen,Minghui Qiu,Yiqun Fan
Ceramic membrane contactors hold great promise for CO2desorption due to their high mass transfer area as well as the favorable characteristics of ceramic materials to resist harsh operating conditions. In this work, a hydrophobic tubular asymmetric alpha-alumina (α-Al2O3) membrane was prepared by grafting a hexadecyltrimethoxysilane ethanol solution. The hydrophobicity and permeability of the membrane were evaluated in terms of water contact angle and nitrogen (N2) flux. The hydrophobic membrane had a water contact angle of ~132° and N2flux of 0.967 × 10−5mol/(m2∙s∙Pa). CO2desorption from the aqueous monoethanolamine (MEA) solution was conducted through the hydrophobic tubular ceramic membrane contactor. The effects of operating conditions, such as CO2loading, liquid flow rate, liquid temperature and permeate side pressure, on CO2desorption flux were investigated. Moreover, the stability of the membrane was evaluated after the immersion of the ceramic membrane in an MEA solution at 373 K for 30 days. It was found that the hydrophobic α-Al2O3membrane had good stability for CO2desorption from the MEA solution, resulting in a <10% reduction of N2flux compared to the membrane without MEA immersion.Keywords:membrane contactor;carbon dioxide;desorption;ceramic membrane
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DALTON TRANSACTIONS
·
2021
·Vol. 51
·期 2
·541-552
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IF 4.39
Dong Fang,Linlin Zhang,Yongjian Niu,Yuanyuan Wang,Qingxiao Su,Jiao Wang,Cheng Wang
SnO2 is one of the most promising catalysts for CO2 electroreduction. However, the intrinsic low electrical conductivity and weak CO2 adsorption and activation capability have rendered the reaction kinetically sluggish and inefficient. To surmount these hurdles, herein, W was incorporated into SnO2 nanosheets to modulate the electronic structures. Compared with pristine SnO2, the p-band centre of W-doped SnO2 was elevated towards the Fermi level, accompanied by the reduction in the band gap and work function. As a result, both the CO2 adsorption and the electron transfer process were promoted, thus lowering the activation energy barrier for CO2 reduction. Benefitting from these, a maximum faradaic efficiency of 87.8% was achieved for HCOOH at −0.9 V vs. the RHE. Meanwhile, the current density and energy efficiency approached 20.92 mA cm−2 and 60%, respectively. Such performances could sustain for 14 h without obvious fading and exceeded pristine SnO2 and most reported Sn-based catalysts. Tafel slope and reaction order analyses further suggested that the reaction proceeded following a stepwise electron–proton transfer pathway with the formation of CO2˙− as the rate determining step. This work demonstrated the effectiveness of electronic structure tuning in promoting the catalytic performances of p-block metal oxides and contributed to the development of efficient catalysts for sustainable energy conversion and carbon neutrality.
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高影响因子
Processes
·
2021
·Vol. 9
·期 12
·2140
·
IF 2.847
Bin Liu,Zhe Cui,Wende Tian
Tertiary amines have been used as alternative absorbents for traditional primary and secondary amines in the process of carbon capture. However, the carbon dioxide (CO2) absorption rates in these kinds of amine are relatively slow, which implies greater investment and construction costs and limits the large-scale application of carbon capture. Carbonic anhydrase (CA) is considered to be an ideal homogeneous catalyst for accelerating the rate of CO2into aqueous amine solution. In this work, CO2absorption combining CA with two single aqueous tertiary amines, namely triethanolamine (TEA) and 2-(diethylamino)ethanol (DEEA), was studied by use of the stopped-flow apparatus over temperature ranging from 293 to 313 K. The concentrations of selected aqueous amine solution and CA used in the experiment were ranging among 0.1–0.5 kmol/m3and 0–50 g/m3, respectively. Compared to the solution without the addition of CA, the pseudo first-order reaction rate in the presence of CA (k0,withCA) is significantly increased. The values ofk0,withCAhave been calculated by a new kinetics model. The results of experimental and calculatedk0,amineandk0,withCAin CO2-amine-H2O solutions were also investigated, respectively.Keywords:carbon capture;CO2absorption;carbonic anhydrase;reaction kinetics
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ACS Applied Nano Materials
·
2021
·
IF 5.097
Chuanhong Wang,Jun Zhang,Zhonggang Wang
Four nonfluorinated and fluorinated nanoporous polymers [PAN-5H, PAN-5F, PAN-2F, and PAN-2(CF3)] were synthesized from a triazine-based tetramine with benzaldehyde, pentafluorobenzaldehyde, 3,5-difluorobenzaldehyde, and 3,5-bis(trifluoromethyl)benzaldehyde, respectively. It is interestingly found that the porosity parameters and selective adsorptions of CO2 and light hydrocarbons strongly depend not only on the number and kind of fluorine atoms and fluorinated groups, but also on the substituted position on the phenyl rings in the fluorinated porous polymers. Relative to PAN-5H and PAN-5F, PAN-2F, and PAN-2(CF3) with phenyls meta-substituted by two fluorinated groups exhibit considerably increased BET surface areas from 502 to 1269 m2/g. At 298 K and 1 bar, the uptakes of C3H8, C2H6, and C2H4 in PAN-2F reach 4.62, 3.64, and 3.20 mmol/g, respectively, whereas PAN-5F exhibits the highest adsorption selectivities of C3H8/CH4 (372.3), C3H8/CO2 (33.2), C2H6/CH4 (21.8), C3H8/C2H6 (9.4), and CO2/CH4 (7.1) among the four polymers. The dynamic breakthrough experiments demonstrate that the mixed gases of C2H6/C2H4, C3H8/CH4, C2H6/CH4, and CO2/CH4 can be separated by the fluorinated polymers under ambient condition. The achieved results are significant for understanding the effects of fluorine-functionalization on the separation of ethylene and CO2 from light hydrocarbons in nanoporous polymers.
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Journal of Materials Chemistry A
·
2021
·Vol. 10
·期 2
·881-890
·
IF 12.732
Peng Hu,Hao Liu,Hao Wang,Jie Zhou,Yongqing Wang,Hongbing Ji
CO2 capture, especially under ultralow-pressure regions (400–10 000 ppm), is extremely essential and challenging to keep the prolonged manual operation in confined spaces and reduce CO2 corrosion in natural gas. Although many MOFs have been covered for CO2 capture, they usually suffered from unheeded morphology engineering associated with diffusion kinetics and unbridgeable CO2 adsorption under ultralow pressure. Herein, we have successfully targeted pyrazine-functionalized Co-MOF (1a′) nanocrystals having dapper hexahedral morphology through skillfully integrating morphology engineering and pore functionality. The yielded 1a′ paradigm with snug pore microenvironment afforded record-high adsorption performance for trace CO2 capture (1.36 mmol g−1 at 400 ppm and 5.7 mmol g−1 at 10 000 ppm), yet eclipsed adsorption behavior for CH4 and N2 at 298 K. The decent pore geometry awarded 1a′ with superior property for CO2/CH4 and CO2/N2 separation, giving higher IAST selectivity (1454 for 15/85 CO2/N2 and 494 for 50/50 CO2/CH4). Besides, 1a′ showed an improved hydrophobic nature, with a desired CO2/H2O uptake ratio of 0.45 and improved diffusion selectivity (DM,CO2/DM,H2O) of 17.7. Breakthrough tests visualized that 1a′ could realize high-purity CO2 (>96%), yielding maximum CO2 productivity (162 and 164.9 litres per kilogram for 18/85 CO2/N2 and 50/50 CO2/CH4). Modeling simulations have cooperatively revealed the structure–property relationship between guest molecules and the framework. This work presents an advanced benchmark adsorbent for low-concentration CO2 capture from flue gas and natural gas.
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Journal of CO2 Utilization
·
2021
·
IF 7.132
Zhongzheng Zhang,Shijian Lu,Guofei Shen,Yonghui Zhao,Tianyang Zhu,Qiang Gao,Nannan Sun,Wei Wei
The rapid synthesis of highly ordered nitrogen-doped mesoporous carbon single crystals with regular and tunable single-crystal morphologies were successfully realized via a controllable co-assembly strategy by using F127 as structure-directing template, 2-methylimidazole as nitrogen source and morphology-adjusting agent, and hexamethylenetetramine as formaldehyde source. Compared with other methods for carbon crystal growth, intricate pre-polymerization steps, taxing synthesis conditions, and long duration time are not requisite for this strategy. Detailed investigation on the effects of 2-methylimidazole dosage, hydrothermal temperature and time, and carbonization temperature on morphology, structure, and nitrogen content of carbon crystals were systematically conducted. Furthermore, one reasonable assembly mechanism was elucidated from both experimental and theoretical perspectives. It was found 2-methylimidazole actively involved in the formation of the polymer matrices via H-bonding to surfactant and chemical reactions with formaldehyde and resorcinol. As such, the introduced 2-methylimidazole not only acted as an effective nitrogen precursor to significantly promote the nitrogen content in resulted crystal carbons, but also served as a positive morphology-tuning agent. Its increasing use successfully achieved the morphology adjustment from hexagonal prisms to rhombic dodecahedrons and then spheres. With intrinsic enriched nitrogen content and large surface area, our synthesized carbon crystals show excellent CO 2 adsorption performance.
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Reaction Kinetics Mechanisms and Catalysis
·
2021
·Vol. 134
·期 2
·823-835
·
IF 2.081
Wang Ying,He Runfa,Wang Cong,Li Gang
A kind of heterogeneous catalyst MCM-41-S-ImBr was prepared by grafting 1-vinyl-3-ethylimidazolium bromide ([VEIM]Br) on the surface of MCM-41. The catalyst was characterized by X-ray diffraction patterns, Fourier transform infrared spectroscopy and element analysis as well as scanning electron microscopy. It showed that [VEIM]Br was successfully grafted on MCM-41 and the catalyst possessed an average particle size of 1.4 µm with intact mesoporous structure. Moreover, the catalyst exhibited high catalytic activity in the cycloaddition reaction of CO 2 with epichlorohydrin without co-catalyst. The conversion of epichlorohydrin was 98.5% and the selectivity of cyclic carbonate was 98.3% at 130 °C under 1.6 MPa for 6 h. Reaction kinetic study indicated that the pseudo-first order rate constant was 0.223 ± 0.001 h −1 . It is proved that MCM-41-S-ImBr could be used at least 4 times without obvious decrease in catalytic performance. A possible reaction mechanism was also proposed: the quaternary imidazolium ion cooperatively worked with the bromide ion to catalyze the reaction. Graphical Abstract
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危险品化学品经营许可证（带存储）