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ENERGY & FUELS · 2020 · IF 3.421

Experimental and Kinetic Study on CaO-based CO2 Sorbent Pellets with Different Binders

Yang Zhang,Xun Gong,Yang Peng,Erwei Leng,Yang Li,Xiaomin Li

In this work, sorbent pellets were prepared based on six synthetic powdery sorbents. CO2 uptake tests and kinetic analysis were carried out to screen sorbent pellets. Experimental results showed that the CO2 capture capacity of sorbent pellets was lower than that of powdery sorbents, which was mainly attributed to reduced Brunauer–Emmett–Teller (BET) specific surface area caused by pore structure damage during the pelletization process. However, the sorbent pellet CaSi75p containing 75 wt % CaO and 25 wt % Ca2SiO4 was less affected by pelletization than other sorbent pellets, which can be explained by the formation of cracks and pores that resulted from the crystalline change of Ca2SiO4 during the calcination–carbonation cycles. Among all of the sorbent pellets, CaSi75p showed the highest CO2 capture capacities of 0.531 g/g and 0.26 g/g in the first and 25th cycles. The performance of sorbent pellets was improved by adding cellulose as a pore-forming material. The reaction rate constants for all sorbents in each cycle were calculated. The experimental and kinetic data indicated that CaSi75p was an excellent sorbent even without adding cellulose.

CAS / MDL: 78-10-4
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MICROPOROUS AND MESOPOROUS MATERIALS · 2020 · IF 4.551

Functionalized ZIF-7/Pebax® 2533 mixed matrix membranes for CO2/N2 separation

Jie Gao,Haizhuo Mao,Hua Jin,Chen Chen,Armin Feldhoff,Yanshuo Li

Membrane-based separation technology has evolved as a competitive approach for CO 2 capture from flue gas (mainly N 2 ). To achieve high separation performance, three partially NH 2 -, OH- and CH 3 OH- functionalized mixed-linker-ZIF-7 were successfully synthesized, and incorporated into polyether-block-amide (Pebax® 2533) polymer to form mixed-matrix membranes (MMMs). As evidenced by the CO 2 adsorption isotherms , introducing functional groups in the ZIF-7 framework was indeed beneficial for CO 2 adsorption. All MMMs composed of ZIF-7-NH 2 , ZIF-7-OH and ZIF-7-CH 3 OH offered better CO 2 /N 2 separation performance than the parent ZIF-7-Pebax® 2533 membrane, suggesting the positive effect of functionalized ZIF-7 fillers on the gas separation performance. Among the three functionalized ZIF-7 based MMMs, the ZIF-7-OH-Pebax MMMs exhibited the best performance for CO 2 /N 2 separation, which might be ascribed to the highest adsorption selectivity of CO 2 over N 2 predicted by ideal adsorbed solution theory (IAST) for ZIF-7-OH fillers. The 14% ZIF-7-OH-Pebax MMM showed high CO 2 permeability of 273 Barrer and CO 2 /N 2 separation factor of 38, which increased by 60% and 145% as compared with the neat Pebax membrane. The strategy of preparing functionalized MOFs with strong affinity for CO 2 provides an effective method to develop MMMs for highly efficient CO 2 separation.

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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2021 · IF 5.816

Catalytic reduction of CO2 by Al–Sn-CNTs composite for synthesizing formic acid

Jinrui Guo,Jing Tian,Jinhua Deng,Xinyu Yang,Binghui Duan,Yong Liu

Electrochemical reduction and photocatalytic reduction of CO 2 have attracted more and more attention, but they also face the problem of low utilization efficiency of electricity and solar energy. In this study, a new strategy of applying a novel Al–Sn-CNTs composite in electrochemical corrosion process was proposed to reduce CO 2 without additional electricity and light. In the Al–Sn-CNTs/CO 2 system, micro galvanic cell with Al as anode and Sn or CNTs as cathode was formed, and CO 2 was reduced to formic acid on the cathode surface . The cumulative formic acid concentration of the Al–Sn-CNTs/CO 2 system achieved 21.18 mg/L within 60 min under the conditions of initial pH 9.0, Cl − concentration 10 mmol/L, and Al–Sn-CNTs composite dosage 2 g/L. Based on the morphology, crystal structure and electrochemical test results of the Al–Sn-CNTs composite, a possible mechanism of CO 2 reduction to formic acid in the Al–Sn-CNTs/CO 2 system was proposed.

CAS / MDL: 7429-90-5 25322-68-3
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Defect-engineering of Zr(IV)-based metal-organic frameworks for regulating CO2 photoreduction

Shi-Qing Wang,Xu Gu,Xinzhu Wang,Xiao-Yu Zhang,Xiao-Yao Dao,Xiao-Mei Cheng,Jing Ma,Wei-Yin Sun

Defects in MOFs can benefit light absorption and charge transfer for photocatalytic application, nevertheless, studies on interplay between structural defects and photocatalytic properties of MOFs are in infancy. Herein, a series of UiO-66-NH 2 with different kinds of defects were created for regulating CO 2 photocatalytic reduction. Theoretical calculations in combination with experimental data verified that the sample with ligand-vacant (UiO-66-NH 2 -LV) defect performed better than non-defect, missing-cluster and monocarboxylate compensated ones in the photocatalytic CO 2 reduction reactions. UiO-66-NH 2 -LV shows superior photocatalytic activity with the highest CO yield of 30.5 μmol g −1 h −1 , which is 9.2 times higher than that of the sample with missing-cluster (UiO-66-NH 2 -MC), as well as the highest quantum yield (QY) of 0.90%. DFT calculations further demonstrate the correlation between discriminative photocatalytic activities in defect structures and tunable electronic properties characterized by absorption energy, E abs , and charge transfer energy, E LMCT , in the photocatalytic process. The ligand-vacant defect with the lowest sum of E abs and E LMCT will lower photocatalytic reaction energy barrier in the rate-limiting step among the elementary reaction step during CO 2 photoreduction. The insights gained from this study will guide the MOFs defect-engineering for enhancing CO 2 photocatalytic capacity.

CAS / MDL: 10026-11-6 102-71-6
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Journal of the Taiwan Institute of Chemical Engineers · 2021 · IF 5.876

Nitrogen and sulfur co-doped porous carbons from polyacrylonitrile fibers for CO2 adsorption

Tingyan Lu,Qian Li,Jiawei Shao,Linlin Wang,Ruixue Pang,Xiaying Wu,Xin Hu

Backgrounds Adsorption by adsorbents is accepted as a promising technology that can efficiently separate CO 2 from flue gas. Optimal adsorption performance can be obtained by specific solid adsorbents with excellent CO 2 adsorption capacity. Methods In this work, N, S co-doped porous carbons were synthesized from polyacrylonitrile fiber by a facile synthesis process i.e. hydrothermal treatment followed by KOH activation. N, S enriched hydrochar was obtained after hydrothermal treatment of polyacrylonitrile fiber and ammonium sulfide. Further KOH activation of hydrochar obtained N, S co-doped carbons with advanced porous structure. Significant findings This series of sorbents has the highest CO 2 uptake of 3.37 and 5.23 mmol g −1 at 1 bar, 25 °C and 0 °C, respectively. Detailed investigation revealed that the mutual effects of narrow microporostiy, N and S content are responsible for the CO 2 uptake of these adsorbents. Additionally, these adsorbents also show various good CO 2 capture properties such as excellent recyclability, reasonable CO 2 /N 2 selectivity, moderate heat of adsorption, fast adsorption kinetics, and good dynamic adsorption capacity. These findings suggest that N, S co-doped porous carbons derived from polyacrylonitrile fiber are potential promising sorbents for CO 2 capture.

CAS / MDL: 12135-76-1
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Highly selective CO2 capture and photoreduction over porous carbon nitride foams/LDH monolith

Biao Zhu,Qianxin Xu,Xiaoyan Bao,Hao Yin,Yumei Qin,Xing-Can Shen

Sunlight-driven photocatalytic CO 2 into useful carbon compounds is an ideal way to mitigate the greenhouse effect. However, this strategy is limited by poor light absorption and rapid photoexcited electron-hole recombination of traditional photocatalysts. Here, a g-C 3 N 4 (CN) foam/LDH heterojunction monolith (NCF) was fabricated by growing NiFe-LDH in situ on the porous CN foam substrate. The composite had good air permeability and light transmittance, which improves light-harvesting, CO 2 capture, and interfaces charge transfer of the NCF. The results show that the NCF catalyst has good CO 2 adsorption performance (1.52 mmol g −1 ) and enhanced CO 2 photoreduction activity (55.1 μmol g -1 h −1 ), which is ∼ 10 times higher than that of pure LDHs powder. Furthermore, the practical applicability of the NCF monolith with different thicknesses is illustrated via the CO 2 photoreduction test for the first time. This work could shed light on the development of dual-functional materials for efficient capture and photoreduction of CO 2 .

CAS / MDL: 12125-01-8 3317-61-1
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CARBON · 2021 · IF 9.594

CsPbBr3 perovskite quantum dots anchored on multiwalled carbon nanotube for efficient CO2 photoreduction

Mengyang Shu,Zhijie Zhang,Zhongliang Dong,Jiayue Xu

Converting CO 2 into valuable fossil fuels through artificial photosynthesis is regarded as an appealing approach to address the problems of global warming and energy crisis, which primarily depends on the development of robust and effective photocatalysts . Herein, we illustrate the construction and fabrication of a multiwalled carbon nanotube (MWCNT)/CsPbBr 3 perovskite quantum dots (QDs) nanocomposite with efficient CO 2 photoreduction activity. In this photocatalytic system, the highly conductive MWCNT acts as an electron acceptor to inhibit the carrier recombination in the CsPbBr 3 QDs. When the content of MWCNT was 4.0 wt%, the resultant CsPbBr 3 /MWCNT exhibited the optimum photocatalytic performance, with the yields of CO and CH 4 3.14 and 2.13 times that of pristine CsPbBr 3 QDs, respectively. The rapid electron extraction and transfer from CsPbBr 3 QDs to MWCNT, as well as the enhanced visible light harvesting ability accounted for the remarkable photocatalytic performance. This work is anticipated to provide new pathway for designing efficient perovskite-based photocatalyst in energy conversion applications.

CAS / MDL: 308068-56-6
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Journal of Energy Chemistry · 2021 · IF 9.676

Tuning the electron structure enables the NiZn alloy for CO2 electroreduction to formate

Xiaodong Zhang,Yajiao Zhou,Hang Zhang,HuangJingWei Li,Kang Liu,Hongmei Li,Hao Pan,Junhua Hu,Junwei Fu,Shanyong Chen,Min Liu

Formate is an important liquid chemical, which can be produced by electrocatalytic carbon dioxide reduction reaction (CO 2 RR). Most of the metal catalysts for CO 2 RR to formate are toxic or noble metals, such as Cd, Hg, Pb and Pd, leading to the environmental pollution or increased production costs. Herein, we develop an environmentally friendly and low-cost NiZn alloy catalyst for CO 2 RR to formate. The X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) confirm the alloy structure of the prepared NiZn catalyst. As for a catalyst for CO 2 RR, the NiZn alloy exhibits the FE HCOO - (Faraday efficiency of HCOO – ) of 36 ± 0.7% at − 0.9 V vs. RHE in 0.1 M KHCO 3 , and remarkable stability for 40,000 s at − 0.8, −0.9, −1.0 and − 1.1 V vs. RHE, respectively. Theoretical calculation results indicate that the NiZn alloy exhibits the middle valence electron structure between the Zn and Ni metal, resulting in the favorable pathway for HCOOH formation but unfavorable for the hydrogen evolution reaction and CO production. The Ultraviolet Photoelectron Spectroscopy results verify the modulated valence electron structure for NiZn alloy as compared to Ni and Zn, consistent with the theoretical calculation results. This work provides new insights into design of alloy catalysts for CO 2 RR to formate.

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FOOD SCIENCE AND BIOTECHNOLOGY · 2021 ·Vol. 30 ·期 10 ·1303-1312 · IF 2.391

Discrimination of Camellia seed oils extracted by supercritical CO2 using electronic tongue technology

Duan Di,Huang Yong,Zou Ying,He Bingju,Tang Ruihui,Yang Liuxia,Zhang Zecao,Su Shucai,Wang Guoping,Zhang Deyi,Zhou Chunhui,Li Jing,Deng Maocheng

Analytical method which combines electronic tongue technique and chemometrics analysis is developed to discriminate oil types and predict oil quality. All the studied Camellia oil samples from pressing, n -hexane extraction and supercritical CO 2 extraction (SCCE), were successfully identified by principal component analysis (PCA) and hierarchical cluster analysis (HCA). Furthermore, multi factor linear regression model (MLRM) was established to predict oil quality, which are indicated by acid value (AV) and peroxide value (POV). The practical potential of e-tongue for the discrimination and assessment of Camellia oils has shown promising application in the characterization of Camellia oils in the oil quality evaluation.

CAS / MDL: 7783-90-6 87-69-4
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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Mixed matrix membranes comprising dual-facilitated bio-inspired filler for enhancing CO2 separation

Xia Lv,Lu Huang,Siyuan Ding,Jiangnan Wang,Long Li,Chao Liang,Xueqin Li

In this work, a novel dual-facilitated bio-inspired zeolitic imidazolate framework (Bio-ZIF) was proposed to simulate the structure and function of carbonic anhydrase (CA), because it can overcome the low stability and high price of the CA. A novel type of mixed matrix membrane (MMM)-composed of Bio-ZIF and Pebax® MH 1657 (Pebax) was fabricated and used to enhance CO 2 separation performance. The bio-inspired active sites of Bio-ZIF can catalyze the reversible hydration of CO 2 in the form of bicarbonate to facilitate the quick transport of CO 2 across the MMMs, increasing CO 2 permeability. Furthermore, the amino groups of Bio-ZIF reacted with CO 2 to produce zwitterion as an intermediate during the reversible reaction, facilitating CO 2 permeation in the MMMs. It can be concluded that Bio-ZIF performed the dual-facilitated functions in the MMMs by reversible hydration and reversible reaction with CO 2 molecules. Thus, the as-prepared MMMs exhibited an excellent CO 2 separation performance. Particularly, Pebax/Bio-ZIF-12 MMM presented an optimal CO 2 permselectivity with CO 2 permeability of 542 ± 6.0 Barrer and CO 2 /CH 4 separation factor of 40 ± 0.4, surpassing the 2008 upper bound. This work provided an ingenious strategy to design bio-inspired fillers to achieve dual-facilitated functions in MMMs for enhancing CO 2 separation.

CAS / MDL: 10196-18-6
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Journal of CO2 Utilization · 2021 · IF 7.132

CO2 hydrogenation on CeO2@Cu catalyst synthesized via a solution auto-combustion method

Bowen Lu,Yongqing Xu,Zewu Zhang,Fan Wu,Xiaoshan Li,Cong Luo,Liqi Zhang

Cu-based catalysts had been widely used in CO 2 hydrogenation process for their excellent performance and high selectivity. Micron-sized Cu powder obtained by ball milling exhibited poor CO 2 activity for its large particle size and small specific surface area, limited its catalytic application. In this work, micron Cu powder was modified with CeO 2 species synthesized from different cerium precursor salts via a solution auto-combustion method to investigate CO 2 hydrogenation activity. This work revealed that CeO 2 species formed from cerium acetate precursor salt achieved excellent CO 2 performance (1.64 mol/g cat .h at 400 °C), which was 3.8 times and 6000 times higher than that from cerium nitrate salt or cerium chloride salt, respectively. Interestingly, a thick dense CeO 2 shell would be formed on micron Cu generated from cerium(III) chloride precursor salt, which inhibited CuO x reduction and had the opposite effect for RWGS reaction. In addition, the CuO x species in CeO 2 @Cu synthesized from cerium chloride salt resulted in the CH 4 selectivity. The enhancement performance of the CeO 2 @Cu prepared from cerium acetate salt and cerium nitrate salt could be attributed to the oxygen defects formed around the Cu-Ox-Ce interface area and metallic Cu in the RWGS reaction. Cerium precursor salts enhanced the structural integrity of CeO 2 @Cu and played a vital role in RWGS reaction. These results will support a new direction for exploring micron Cu powder in Cu-based catalysts for CO 2 utilization.

CAS / MDL: 40503-90-0 4210-60-0
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ChemCatChem · 2021 ·Vol. 13 ·期 23 ·4931-4936 · IF 5.686

Hierarchical Bimetallic Electrocatalyst with Amorphous SnO Layer for Highly Efficient Electroreduction of CO2

Cuizhu Huo,Xinxing Cao,Zixian Ye,Yu Li,Tongbu Lu

Graphical Foam supported : The hierarchical bimetallic electrocatalyst comprising Cu foam-supported bundle-like structure with thin amorphous SnO shell (Sn-24 h@CB) was successfully synthesized for highly efficient electrocatalytic reduction of carbon dioxide. An unprecedented partial current density of C1 products (CO and HCOOH) up to 128.6 mA cm −2 was achieved with a Faradaic efficiency of ∼80 % in H-type cell. Renewable electricity-driven reduction of CO 2 into value-added chemicals has been recognized as a promising sustainable energy conversion method to achieve carbon-neutrality. Although Sn-based catalysts show excellent selectivity towards CO and HCOOH in CO 2 reduction, the reaction activity, i. e. current density, remains quite low (<100 mA cm −2 ). Herein, a hierarchical bimetallic electrocatalyst consisting of Cu foam-supported bundle-like structure and thin amorphous SnO layer was fabricated for efficient electroreduction of CO 2 to C1 products (CO and HCOOH). The hierarchical structure ensured higher large electrochemically active surface area, while the thin amorphous SnO layer could efficiently adsorb CO 2 , and stabilize the *CO 2 − intermediate formed in the rate-determining step, thereby boosting the reaction activity of CO 2 reduction. As a result, an unprecedented partial current density of 128.6 mA cm −2 was achieved for C1 products at −1.4 V vs. RHE with a Faradaic efficiency of 79.2 % in an H-type cell. The strategy of integrating optimized structure with active site here may be beneficial to other related energy conversion systems.

CAS / MDL: 298-14-6 10025-69-1
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