Journal of CO2 Utilization
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2023
·
IF 7.7
Shibo Yuan,Peng Bai,Yi He,Jiafa Chen,Yicheng Zhao,Yongdan Li
Photocatalytic N-formylation of amines with CO 2 is a promising strategy to convert CO 2 into value-added chemicals sustainably. In this work, a black TiO 2 -supported Cu photocatalyst is prepared through a solvothermal method for the N-formylation of N-methylaniline with NaBH 4 as the reducing agent. Cu nanoparticles and oxygen vacancies are formed on the surface of the photocatalyst after reduction with H 2 , which decreases the band-gap energy and promotes the separation of photogenerated electrons and holes, thereby improving the photocatalytic activity remarkably. A 100 % conversion is achieved after 9 h radiation, and the yield of N -methylformanilide reaches 81 %. Both the amount of NaBH 4 and the pressure of CO 2 show important influences on the activity and selectivity of the photocatalytic process, and the carbon and hydrogen in the aldehyde group are from CO 2 and NaBH 4 , respectively. The photocatalyst also shows promising cycling durability.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Ting Liang,Jingwen Wei,Shiming Zhang,Jinhang Yang,Jiangli Sun,Zuji Li,Zhihong Li,Zebin Yu,Shuangfei Wang,Yanping Hou
Design of photocatalysts with high-efficiency for sunlight utilization is one of the prerequisites for CO 2 photoreduction . Besides, modulating a stable electron-donating environment to meet the energy barrier for CO 2 reduction to CO is crucial. In this work, the ZnSe/Ag 2 Se/AgBr (ZAA) heterojunction was fabricated by growing the ZnSe on the AgBr surface accompanied by in-situ generation of Ag 2 Se between the two components by hydrothermal process. Results showed that the ZAA exhibited excellent light response ability over the full wavelength range. X-ray photoelectron spectroscopy (XPS) and electron spin resonance (ESR) demonstrated that the charge transfer of the ZAA conformed to dual Z-scheme mechanism, with the Ag 2 Se acting as an electron transfer bridge, which in turn acted as an electron reservoir to accelerate electron transfer, facilitating carriers’ separation. The highest CO yield of 54.14 µmol/g/h was obtained from the optimal ZAA-2, which was 11.76 and 10.44 times of pure ZnSe and Ag 2 Se, respectively. This work demonstrated the feasibility of a dual Z-scheme heterostructure with full spectrum response for offering stable electron-donating environment and improving electron transfer for enhanced photocatalytic activity.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Shaoqi Zhang,Haiyang Yu,Yi Wang,Yuxiang Yan,Jun Dai,Dajun Shu,Xinglong Wu
CO2 possesses extraordinary thermodynamic stability, and its reduction reaction involves multiple electron-transfer processes. Thus, high-density electron occupation on a catalyst surface is an effective driving force for improving the photocatalytic activity. Here, we report on the fabrication of Fe-doped Bi2O3 catalysts (denoted as FexBi2-xO3) with different Fe contents using the solvothermal method. The self-assembled catalyst has a nanoflower-like morphology, and its performance of CO2 reduction to CO is improved largely dependent on the Fe content. In the sample with a 7.0% Fe content (Fe0.07Bi1.93O3), the CO evolution rate reaches 30.06 μmol g–1 h–1, which is about 6 times higher than the 4.95 μmol g–1 h–1 of pristine Bi2O3, and shows excellent photostability after three cycles, with each cycle lasting for 7 h. Theoretical calculation and spectral characterization reveal that such a good CO2 reduction reaction performance arises from effective surface occupation of Fe, which not only enhances sunlight absorption but also significantly increases the surface electron density on the double metal active sites. This work provides a new strategy for improving the photocatalytic performance by surface metal doping in some metal oxide photocatalysts.
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ChemistrySelect
·
2023
·Vol. 8
·期 13
·e202202681
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IF 2.1
Qing-Qing Pang,Xi-Zheng Fan
Graphical The ultra-fine Pd nanoparticles (NPs) are constructed by strong electrostatic adsorption strategy to ensure ample active sites, further enhance the light absorption intensity and optimize the separation efficiency of electron and hole, contributing to dramatically promote the performance of photocatalytic CO 2 reduction and stability in the gas-solid phase system. The photocatalytic CO 2 converted into the value-added products is regarded as a green strategy for the conversion and utilization of energy. Herein, we develop a commodious SEA (strong electrostatic adsorption) strategy to synthesize Pd-based photocatalysts with ultra-fine Pd NPs (Pd/TiO 2 −S−B). As verified by experiments and characterizations, the ultra-fine Pd NPs can inexorably heighten the reaction activity of catalyst, because it can provide several functions consist of improving the carrier separation efficiency, light absorption and CO 2 molecules adsorption. Meanwhile, the interaction of Pd and substrate can prevent the agglomeration of Pd NPs in reaction process. The designed Pd/TiO 2 −S−B contributes excellent performance in a gas-solid system. The yields of CO (105.1 μmol/g-cat) and CH 4 (254.3 μmol/g-cat) detected, are about 5.25 and 6.24-fold higher than those of pristine TiO 2 . Pd/TiO 2 −S−B also exhibits the forceful stability with acceptable decline of catalytic activity after three cycles. This opens the door for the preparation of high-performance and steady photocatalysts by reliable and effortless strategies toward CO 2 reduction.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Jian Yang,Zhilong Zhou,Peng Lu,Min Wu
The preservation of fresh fruit and vegetables is always a challenge. Equilibrium modified atmosphere packaging (EMAP) is ideal for preserving fresh produce. The gas transmission and selectivity of EMAP films is crucial for achieving atmospheric equilibrium in packaging. Inspired by leaf porous structure regulating their gas exchange function, we selected natural porous diatomite as the gas channel and modified it with polyethyleneimine (PEI). By introducing diatomite into the film matrix of CNFs, the gas transmission and CO 2 /O 2 selectivity of EMAP films were regulated. The atmosphere in all the packages of EMAP films reached equilibrium within 24 h, which kept the fruit in low intensity aerobic respiration. The EMAP film of D g P 7.5 (O 2 transmission rate 43.33 cc m −2 day −1 bar −1 , CO 2 /O 2 selectivity 1.56) was found to be the most suitable for packaging litchis and green plums. Diatomite with porous structures will provide a design concept for EMAP films.
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MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2023
·Vol. 224
·期 18
·2300036
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IF 2.5
Wei Zhang,Yi Sun,Yiting Xu,Xiaobo Yu,Yajin Fang,Fei Liu,Haining Na,Jin Zhu
Fabrication of fluorescent cellulose with aggregation-induced emission (AIE) characteristics is usually achieved by grafting tetraphenylethylene (TPE) to the cellulose backbone using TPE derivatives with highly active functional groups such as carboxylic, isothiocyanate, and alkynyl groups. However, besides the complicated synthetic routes of these TPE derivatives, conversion of hydroxyl groups in the cellulose chain to more reactive groups such as amine or azide groups is usually involved, and the resulting products have a degree of substitution (DS) of TPE lower than 0.08. Herein, a facile one-pot strategy for the grafting of a TPE group to the cellulose backbone with high DS of up to 0.22 in a CO 2 switchable solvent under mild reaction conditions is reported. The hydroxyl groups in the cellulose are in situ converted to cellulose carbonate intermediately during the dissolution step. Subsequently, nucleophilic substitution between the intermediate and a halogenated TPE derivative with bromine atom as leaving group is carried out to achieve the effective grafting of TPE. The synthetic route for this promising TPE derivative is much more convenient than those of TPE derivatives reported in previous studies. This work suggests a new and facile pathway for the synthesis of high-emission fluorescent cellulose with AIE functionality.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Yi Li,Yanghan Chen,Tao Chen,Guoqiang Shi,Lin Zhu,Ye Sun,Miao Yu
Ethanol (C2H5OH) is an economically ideal C2 product in electrochemical CO2 reduction. However, the CO2-to-C2H5OH conversion yield has been rather low and the underlying catalytic mechanism remains vague or unexplored in most cases. Herein, by decorating small Cu2S nanocrystals uniform ly on Cu nanosheets, three desirable features are integrated into the electrocatalyst, including a relatively high positive local charge on Cu (Cuδ+), abundant interfaces between Cuδ+ and zero-valence Cu0, and a non-flat, stepped catalyst surface, leading to the promoted affinity of *CO, decreased *COCO formation barrier, and thermodynamically preferred *CH2CHO-to-*CH3CHO conversion. As a result, a high partial current density of ∼20.7 mA cm–2 and a Faraday efficiency of 46% for C2H5OH are delivered at −1.2 V vs reversible hydrogen electrode in an H-cell containing a 0.1 M KHCO3 solution. This work proposes an efficient strategy for the high-yield CO2-to-C2H5OH conversion, emphasizing the promise for the industrial production of alcohol and related products from CO2.
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ENERGY
·
2023
·
IF 9
Liang Xu,Qi Li,Matthew Myers,Xiaomin Cao
Huff-n-puff methods using nanofluid and/or CO 2 are most promising methods for enhancing oil recovery in the Mahu Oilfield, Xinjiang, China. Six tight glutenite reservoir samples were conducted the huff-n-puff experiment using different displacement fluids (i.e. D 2 O, supercritical CO 2 and nanofluid) following saturation with oil. The results of T 2 NMR spectra of the samples show that D 2 O can readily enter the larger pores stripping the oil with smaller pores remaining relatively untouched. Furthermore, the oil recovery was initially fast before quickly tapering with the final average oil recovery over samples using D 2 O huff-n-puff alone being only 14.89%. However, CO 2 could effectively enter both small and large pores with the oil recovery efficiency from small pores being greater than 20% and from the large pores being even higher with the final average recovery over two samples using CO 2 huff-n-puff alone being 40.44%. Relative to D 2 O alone, the nanofluid improved the oil recovery in small pores by more than 10%. There appears to be a synergistic effect combining CO 2 and nanofluid huff-n-puff; both CO 2 followed by nanofluid huff-n-puff or nanofluid followed by CO 2 huff-n-puff achieved similar final recoveries close to 50% of the overall oil.
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Advanced Materials Interfaces
·
2023
·Vol. 10
·期 12
·2202524
·
IF 5.4
Lei Wang,Xianying Bai,Yawei Gu,Xinxin Shi,Shilong Wang,Jingxian Hua,Rujing Hou,Chongqing Wang,Yichang Pan
2D metal–organic frameworks are attractive filler in mixed matrix membranes (MMMs) due to the high aspect ratio and contact opportunity at the filler–polymer interface. However, their alignment in polymer matrix remains a challenge to fully play their functions. Herein, to our best knowledge, for the first time, the facile synthesis of KAUST-7-NH 2 (KAUST, King University of Science and Technology) nanoplate is reported with 1D channels with an aspect ratio greater than 30. The nanoplates are incorporated and aligned in the 4,4′-(hexafluoroisopropylidene) diphthalic anhydride-2,4-diaminomesitylene (6FDA-DAM) polymer matrix under the shear force with a filler loading up to 50 wt%. The large difference in adsorption abilities between CO 2 and CH 4 from the (001)-oriented KAUST-7-NH 2 nanoplate-based MMMs and the favorable interaction at the filler–polymer interface contribute to the excellent CO 2 /CH 4 separation performance. The resultant membranes show CO 2 /CH 4 selectivity with 66.2% enhancement (surpassed 2008 Robeson upper bound), antiplasticization up to 17 bar, and long-term stability up to 240 h indicating its good potential for natural gas treatment.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Meilin Yin,Lipeng Wang,Shaokun Tang
Rationally integrating desired functional components into a composite material can endow the tailored function to achieve the corresponding purpose. This is the first case where a series of [AeImBr]X%-TAPT-COFs (X = 0, 17, 33, 50, 67, 83, 100) were fabricated by chemically integrating the amino-functionalized imidazole ionic liquid (NH2-IL) onto channel walls of mesoporous covalent organic framework materials ([HO]X%-TAPT-COFs). By virtue of the polar groups (amino groups) and abundant imidazole cations of NH2-IL and its microporous nature, the obtained [AeImBr]X%-TAPT-COFs exhibit higher CO2 capture activity than [HO]X%-TAPT-COFs. Correspondingly, the CO2 equilibrium capture capacity increases from 62.6 to 117.4 mg/g, which is crucial to the storage of enough CO2 around the catalytic active sites. Additionally, the synergistic effect of −NH2 and Br– in NH2-IL can also improve the cycloaddition reaction rate. The characteristics of [AeImBr]X%-TAPT-COFs contribute to the efficient generation of cyclic carbonate through heterogeneously catalyzing CO2-epoxide cycloaddition without any solvents and cocatalysts. Specifically, [AeImBr]83%-TAPT-COF has a CO2 equilibrium capture capacity of 117.4 mg/g and cyclochloroallyl carbonate yield of 99.1%. As a result of the use of the chemical grafting method, [AeImBr]X%-TAPT-COFs possess excellent stability and cycle life. The equilibrium capture capacity and cyclochloroallyl carbonate yield reach 112.7 mg CO2/g adsorbent and 95.0% at the eighth cycle.
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ChemSusChem
·
2022
·Vol. 16
·期 5
·e202201956
·
IF 9.14
Xiu Xing,Yan Liu,Ru-De Lin,Yang Zhang,Zhong-Liu Wu,Xiao-Qi Yu,Kun Li,Na Wang
Graphical Tailor made ! An environmentally friendly and highly effective semi-artificial photosynthetic system (FDH@Rh-TCPP-UiO-66-NH 2 ) was developed for transforming CO 2 into formic acid. The incorporation of NADH-dependent formic acid dehydrogenase (FDH), photosensitive porphyrin ligands and Rh complex lead to highly selective and recyclable system. Herein, a Zr-based dual-ligand MOFs with pre-installed Rh complex was employed for NADH regeneration in situ and also used for immobilization of formic acid dehydrogenase (FDH) in order to realize a highly efficient CO 2 fixation system. Then, based on the detailed investigations into the photochemical and electrochemical properties, it is demonstrated that the introduction of the photosensitive meso-tetra(4-carboxyphenyl) porphin (TCPP) ligands increased the catalytic active sites and improved photoelectric properties. Furthermore, the electron mediator Rh complex, anchored on the zirconium-based dual-ligand MOFs, enhanced the efficiency of electron transfer efficiency and facilitated the separation of photogenerated electrons and holes. Compared with UiO-66-NH 2 , Rh-H 2 TCPP-UiO-66-NH 2 exhibits an optimized valence band structure and significantly improved photocatalytic activity for NAD + reduction, resulting the synthesis of formic acid from CO 2 increased from 150 μg mL −1 (UiO-66-NH 2 ) to 254 μg mL −1 (Rh-H 2 TCPP-UiO-66-NH 2 ). Moreover, the assembled photocatalyst-enzyme coupled system also allows facile recycling of expensive electron mediator, enzyme, and photocatalyst.
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ACS Omega
·
2022
·
IF 4.132
Xia Wang,Wulan Zeng,Xiangjun Kong,Chunling Xin,Yani Dong,Xiude Hu,Qingjie Guo
To achieve the “double carbon” (carbon peak and carbon neutrality) target, low-cost CO2 capture at large CO2 emission points is of great importance, during which the development of low-cost CO2 sorbents will play a key role. Here, we chose peanut shells (P) from crop waste as the raw material and KOH and K2CO3 as activators to prepare porous carbons by a simple one-step activation method. Interestingly, the porous carbon showed a good adsorption capacity of 2.41 mmol/g for 15% CO2 when the mass ratio of K2CO3 to P and the activation time were only 0.5 and 0.5 h, respectively, and the adsorption capacity remained at 98.76% after 10 adsorption–desorption cycle regenerations. The characterization results suggested that the activated peanut shell-based porous carbons were mainly microporous and partly mesoporous, and hydroxyl (O–H), ether (C–O), and pyrrolic nitrogen (N-5) functional groups that promoted CO2 adsorption were formed during activation. In conclusion, KOH- and K2CO3-activated P, especially K2CO3-activated P, showed good CO2 adsorption and regeneration performance. In addition, not only the use of a small amount of the activator but also the raw material of crop waste reduces the sorbent preparation costs and CO2 capture costs.
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