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APPLIED CATALYSIS B-ENVIRONMENTAL · 2022 · IF 24.319

Self-assembled lead-free double perovskite-MXene heterostructure with efficient charge separation for photocatalytic CO2 reduction

Zhipeng Zhang,Bingzhe Wang,Hai-Bing Zhao,Jin-Feng Liao,Zi-Chun Zhou,Tanghao Liu,Bingchen He,Qi Wei,Shi Chen,Hong-Yan Chen,Dai-Bin Kuang,Ying Li,Guichuan Xing

Lead-free double perovskites with superior stability have been considered as promising non-toxic substitutes to their lead-contained counterparts in photocatalysis . However, the severe charge recombination greatly restricts their potential as high-performance photocatalysts. Herein, for the first time, we present a self-assembled heterostructure of lead-free double perovskite Cs 2 AgBiBr 6 nanocrystals (NCs) on the surface of MXene nanosheets via mutual electrostatic attraction. The presence of MXene nanosheets effectively promotes the formation of free charge carriers in Cs 2 AgBiBr 6 NCs via reducing the exciton binding energy. Additionally, the ultrafast photogenerated electron transfer from Cs 2 AgBiBr 6 to MXene with a timescale of 1.1 ps largely prolongs the charge carrier lifetime by two times. As a result of the efficient charge separation and electron extraction, the Cs 2 AgBiBr 6 /MXene heterostructures achieve a high photoelectron consumption yield of 50.6 µmol g −1 h −1 for photocatalytic CO 2 reduction, which surpasses most previously reported lead-free perovskite-based catalysts.

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ENERGY · 2022 · IF 8.857

A novel preparation of solid amine sorbents for enhancing CO2 adsorption capacity using alumina-extracted waste

Xiangyu Li,Zhiqing Wang,Zheyu Liu,Ru Feng,Shuangshuang Song,Jiejie Huang,Yitian Fang

A “wet gel impregnation” method (WGI) was applied to prepare modified CO 2 sorbents derived from alumina-extracted residue of coal ash (AR). Tetraethylene pentamine (TEPA) was selected as an amine polymer and it was evenly dispersed on the surface of AR. And the effects of loading amount, impregnation method, and adsorption temperature on CO 2 adsorption capacity of the sorbent were investigated by thermogravimetric analyzer (TGA). The results showed that the desired sorbent with 60% TEPA loading via WGI had the maximum CO 2 adsorption capacity of 3.45 mmol/g under 100% CO 2 at 75 °C. This was attributed to the fact that the loading in wet gel state dramatically improved TEPA dispersion on the supports and increased the saturated loading of amine. Moreover, the sorbent still maintained stable CO 2 uptake after five repeated adsorption-desorption cycles. These results suggested that amine-impregnated AR sorbent synthesized by WGI was an excellent and low-cost sorbent for CO 2 capture.

CAS / MDL: 112-24-3
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

An MOF-tailored hierarchical porous microenvironment for CO2 as an efficient filler for mixed matrix membranes

Minmin Gou,Ruili Guo,Hengheng Cao,Weifang Zhu,Fu Liu,Zhong Wei

Mixed matrix membranes (MMMs) for separating CO 2 /CH 4 mixture were prepared through incorporating Cu@Al(bpydc) into a Pebax polymer in which Cu@Al(bpydc) synthesized through a competitive coordination method achieved a controllable micro/mesopores structure and abundant functional sites for CO 2 . The hierarchical pores of Cu@Al(bpydc) provided multidimensional diffusion channels in the Pebax matrix, which increased the diffusion of CO 2 . In addition, the abundant chemical groups, such as the polar group COO – and nitrogen Lewis basic groups, created a microenvironment with multiple CO 2 affinity sites in the membrane, increasing the selectivity of CO 2 . A MMM loaded with 5 wt% Cu@Al(bpydc) exhibited excellent CO 2 separating property under wet mixed-gas test conditions. In particular, the CO 2 permeability and selectivity of the MMMs were increased by 92.90% and 27.10% respectively, compared with those of pure Pebax, showing exceptional potential for the separation and capture of CO 2 from biological natural gas.

CAS / MDL: 7784-13-6 1802-30-8
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2022 · IF 24.319

Highly selective photocatalytic reduction of CO2 to ethane over Au-O-Ce sites at micro-interface

Jixiang Ji,Ruru Li,Hao Zhang,Yingnan Duan,Qian Liu,Haozhi Wang,Zhurui Shen

To date, the efficient photocatalytic conversion of CO 2 into high-value C2 products remains a great challenge. Herein, the Au-CeO 2 nanocomposite with Au-O-Ce sites at the micro-interface was developed to achieve a highly selective conversion of CO 2 into C 2 H 6 . This can be partially ascribed to the formation of key intermediates of COCO* was confirmed via in-situ Fourier transform infrared (FTIR) spectroscopy, indicating that the Au-CeO 2 micro-interface could prompt the multi-electron reduction of CO* before desorption, and enable the production of C2 species. Moreover, theoretical calculations suggested that Au-O-Ce sites at the micro-interface could reduce the energy barriers for the formation of COOH* and COCO*, facilitating the production of C 2 H 6 . Therefore, the Au-CeO 2 nanocomposite exhibited a C 2 H 6 production rate of 11.07 µmol g −1 h −1 and high electron selectivity of 93.1 % (product selectivity: 65.3 %), which is comparable with most state-of-the-art photocatalysts.

CAS / MDL: 13463-67-7 12065-65-5
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Tailoring and properties of a novel solar energy-triggered regenerative bionic fiber adsorbent for CO2 capture

Wei Lu,Xiaoyu Shi,Hang Zhou,Wenlu Luo,Lei Wang,Hui He

Using renewable solar energy sources instead of heat energy to desorb CO 2 from adsorbents is a promising strategy for reducing the energy consumption of adsorbent regeneration. However, the photothermal temperature of adsorbents with high CO 2 adsorption capacity cannot desorb CO 2 efficiently in a real sunlight environment. Here, a novel solar energy-triggered regenerative bionic fiber adsorbent for CO 2 capture was designed via bionic electrostatic and chemical cross-linking assembly of cellulose nanofibers, thermosensitive polymer poly(N-isopropylacrylamide), nano-graphene oxide and polyethyleneimine. Excellent photothermal transformation characteristics, thermosensitivity and high density of amino adsorption sites were synchronously endowed onto cellulose nanofibers with hydroxyl groups. The thermosensitivity and hydroxyl synergy of the adsorbent enables it an ultralow regeneration temperature (60 °C) by preventing the formation of refractory urea. Interestingly, the adsorbent possesses a high CO 2 adsorption capacity (6.52 mmol/g) and can be efficiently regenerated by using renewable solar energy, indicating that it is a promising strategy for greatly reducing the energy consumption for adsorbent regeneration.

CAS / MDL: 9002-98-6 106-89-8
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Study on regeneration characteristics of choline chloride-monoethanolamine deep eutectic solvent after capturing CO2 from biogas

Qun Huan,Yan Zhang,Haryo Wibowo,Zhang Xu,Ekkachai Kanchanatip,Li Zhong,Mi Yan

Choline chloride-monoethanolamine deep eutectic solvent (ChCl-MEA DES) can deeply remove CO 2 from biogas. This study focused on regeneration of ChCl-MEA DES after CO 2 capture. The effects of regeneration temperature, time and water content on CO 2 absorption capacity, absorption rate and CO 2 /CH 4 absorption selectivity after regeneration were evaluated. The addition of HZSM-5 catalyst during regeneration further promoted regeneration efficiency. FTIR and NMR indicated that carbamates were formed after absorption, and water made it easier for the amino group to react with CO 2 to form carbamates. The highest regeneration percentage of absorbent was up to 99.89%, and the CO 2 absorption capacity even didn’t decrease significantly after 8 cycles. The ideal regeneration energy consumption in the experiment was also evaluated. This research provided a valuable reference for the application of this absorbent in CO 2 purification of biogas.

CAS / MDL: 67-48-1 142-58-5
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2022 · IF 4.326

Study of Direct Synthesis of DMC from CO2 and Methanol on CeO2: Theoretical Calculation and Experiment

Daoyun Zhu,Haiou Liu,Yangqiang Huang,Xiao Luo,Yu Mao,Zhiwu Liang

Rare earth metal oxides are known to have good catalytic effectiveness in the direct synthesis of dimethyl carbonate (DMC) from CO2 and methanol. In this work, we screened ceria (CeO2) catalysts by analyzing their capacity for CO2 adsorption. The effects of the crystal surface morphology and oxygen vacancy on the catalytic performance of the ceria catalyst were studied by using density functional theory (DFT). The results show that the (110) surface and higher oxygen vacancy content can better promote the synthesis of DMC and that the rod-shaped CeO2 catalyst has a better catalytic effect. The oxygen vacancy content on the catalyst was improved by freeze-drying and confirmed by thermogravimetric analysis, Raman spectroscopy, and electron paramagnetic resonance. The freeze-dried CeO2 (CeO2-FD) then showed a higher catalytic performance. The conversion rate of methanol and the yield of DMC were 33.95% and 584 mmol g–1cat, respectively, under mild conditions (140 °C and 1 MPa).

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JOURNAL OF APPLIED POLYMER SCIENCE · 2022 ·Vol. 139 ·期 30 ·e52661 · IF 3.057

Incorporation of CO2-polyols into ester-based waterborne polyurethane: An effective strategy to improve overall performance

Hongming Zhang,Guangping Han,Wanli Cheng,Shunjie Liu,Xianhong Wang

Amorphous structural CO 2 -polyol was used to modify ester-based water-borne polyurethanes (WPUs), resulting in improved low temperature film forming and comprehensive hydrolysis/oxidation resistance properties. Excellent intact films can be easily formed even at 3°C by adding 5% CO 2 -polyol into the ester-based WPUs (namely PU 5 CO 2 ). Moreover, WPUs modified by CO 2 -polyol show superior hydrolysis/oxidation resistance properties than that of control samples based on castor oil or poly(propylene oxide) glycol. PU 5 CO 2 showed significantly enhanced retention tensile strength from 40% to 68.2% than that of pure ester-based WPU after 5 h immersion in 1.5% NaOH solution, indicating an improved hydrolysis resistance. In addition, the PU 5 CO 2 displayed boosted oxidation resistance property with retention strength increased from 39% to 65%. Notably, the all-around aging resistance of ester-based WPUs intensified with an increase of CO 2 -polyol content. This work indicates that the CO 2 -polyol may be a promising modified material to improve comprehensive hydrolysis/oxidation resistance and low temperature film forming for ester-based WPUs.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Rational fabrication of ZIF-8 forests via metal template-guided growth for promoting CO2 chemical transformation

Xi Liu,Meili Ding,Pan Ma,Chengyuan Duan,Jianfeng Yao

Construction of macroscopic metal–organic frameworks (MOFs) with high processability is crucial for their practical usage. Here, we demonstrate a facile metal template-guided growth approach that exploits the synthesis of forest-like ZIF-8-based material. The 3D self-supported array architecture endows the resultant ZIF-8 forests with efficient exposure of active sites, rapid mass transfer and simple recovery. Under mild catalytic reaction conditions (1 bar CO 2 , 60 ℃), ZIF-8 forests show remarkable activities toward the coupling of epoxides and CO 2 with an excellent cyclic carbonate yield of 96%, surpassing the powdered ZIF-8 crystals. Importantly, the catalytic performance can be well-maintained even after 10 cycles and under both simulated flue gas conditions and full-spectrum light irradiation, demonstrating the potential for practical catalysis. Our work provides a practical guideline to produce macroscopic MOF-based materials with great potential for industrial catalysis.

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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Synergy of nitrogen vacancies and Fe2P cocatalyst on graphitic carbon nitride for boosting photocatalytic CO2 conversion

Xiangli Shi,Pengfei An,Qiong Zhang,Qi Song,Deli Jiang,Dan Tian,Di Li

Photocatalytic CO 2 conversion into value-added chemicals is a promising strategy to remedy the energy crisis and environmental pollution, yet developing cost-effective photocatalysts that can efficiently and selectively convert CO 2 to desirable products is still a great challenge. Herein, we construct a Fe 2 P nanoparticles decorated on the surface of the nitrogen vacancies (NVs) modified g-C 3 N 4 nanosheet hybrid photocatalyst (Fe 2 P/NVsCN) for photocatalytic conversion of CO 2 to CO. The NVs can significantly improve the visible light absorption due to the formation of midgap state, and the metallic Fe 2 P as the cocatalyst is beneficial to promote the photo-generated charge separation and migration, impede the side reaction, in which improve the activity and selectivity. By adjusting the contents of Fe 2 P and NVsCN, the optimal 20%-Fe 2 P/NVsCN(1:5) sample shows an excellent CO evolution rate in visible light of 22.48 µmol g -1 h −1 with 97.5% selectivity, which is superior to most reported g-C 3 N 4 -based photocatalysts. Furthermore, this photocatalyst also exhibits good stability due to the timely consumption of electrons, and it maintains stable CO evolution rate over 20 h. This work opens a new horizon for design and construction of active photocatalyst with high selectivity by synergistic modulating the surface vacancy and cocatalyst.

CAS / MDL: 7778-80-5
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Catalysis Science & Technology · 2022 ·Vol. 12 ·期 20 ·6155-6162 · IF 6.177

Localized surface plasmon resonance effect enhanced Cu/TiO2 core–shell catalyst for boosting CO2 hydrogenation reaction

Lizi Shi,Huimin Liu,Shangbo Ning,Jinhua Ye

Photothermal catalysis is a promising strategy for converting CO2 into high value-added chemical feedstocks. Its current major challenges lie in improving CO2 conversion efficiency and product selectivity. In this work, a series of Cu/TiO2 core–shell catalysts were prepared using the hard template method. The Cu10/TiO2 catalyst exhibited excellent performance for the photothermal conversion of CO2 to CO in the presence of H2 under Xe lamp irradiation (CO2 conversion, 30.6%; CO selectivity, ∼100%; CO maximum yield, 87.1 mmol h−1 gcat−1). Results indicated that the Cu/TiO2 catalyst has a good photo-to-thermal conversion ability based on the significant LSPR effect, and the existence of hot electrons makes the reaction follow the carbonate pathway efficiently. This article successfully achieves efficient CO2 reduction under inexpensive and non-toxic conditions. In addition, it also provides unique insights into the study of the LSPR effect in the field of photothermal catalysis.

CAS / MDL: 5593-70-4
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Boosting the CO2/N2 selectivity of MMMs by vesicle shaped ZIF-8 with high amino content

Rui Ding,Ziheng Li,Yan Dai,Xiangcun Li,Xuehua Ruan,Jiaming Gao,Wenji Zheng,Gaohong He

The amino functionalization of MOFs has been verified to be effective in improving the selective permeation of CO 2 . However, the introduction of amino groups into ZIF-8 by mixed ligands strategy is hard to achieve due to the high steric hindrance of benzene ring in 2-aminobenzimidazole ligand, resulting in insufficient content of amino groups. Therefore, in this work, polystyrene-acrylate (PSA) template is proposed to provide abundant adsorption and reaction sites for the rapid synthesis of NH 2 -ZIF-8 with high content of 2-aminobenzimidazole. Furthermore, the incomplete etching strategy is used to construct PSA modified hollow NH 2 -ZIF-8 nanospheres (PHNZ). Importantly, the thickness of PSA layer and the hollow size are adjusted by the etching time, as revealed by the SEM and TEM images. In this PHNZ, the modified PSA can provide good interface compatibility between PHNZ and Pebax matrix to enhance the CO 2 selectivity, while the hollow structure can reduce the mass transfer resistance and improve the gas permeability. Moreover, the introduced amino groups can enhance the CO 2 affinity of PHNZ and further improve the CO 2 /N 2 selectivity of the PHNZ-based mixed matrix membranes (MMMs). Benefiting from the synergy of good interface compatibility and enhanced CO 2 affinity from the amino groups, the PHNZ/Pebax MMMs present greatly improved CO 2 /N 2 selectivity in contrast with pure Pebax and NH 2 -ZIF-8 based membranes. Besides, as the etching time increases, the PHNZ-2 and PHNZ-3 based MMMs present a higher CO 2 permeability than that of NH 2 -ZIF-8 based MMM, revealing the significance of the hollow structure. The PHNZ-2/Pebax MMM with filler loading of 10 wt% expresses the best gas separation performance with the CO 2 permeability of 121.9 Barrer and CO 2 /N 2 selectivity of 96.6, respectively, showing an increase of 54.7 % and 98.0 % in contrast with pure Pebax membrane. Meanwhile, this CO 2 separation performance is far beyond the Robeson upper bound in 2008 and close to the McKeown upper bound in 2019, demonstrating that the proposed PHNZ displays a promising and competitive potential in MMM based CO 2 capture.

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