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ENERGY & FUELS · 2020 · IF 3.421

Monoethanolamine-Modified Attapulgite-Based Amorphous Silica for the Selective Adsorption of CO2 from Simulated Biogas

Qinglin Li,Hairong Zhang,Fen Peng,Can Wang,Hailong Li,Lian Xiong,Haijun Guo,Xinde Chen

Biogas upgrading technology is important for increasing the heating value of biogas through selective adsorption of CO2. In this work, a series of new monoethanolamine (MEA)-modified attapulgite (ATP)-based amorphous silica (a-SiO2) sorbents with a large surface area and oxygen vacancies were prepared by the impregnation method for the selective adsorption of CO2 from simulated biogas. Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), and N2 adsorption–desorption results indicated that MEA with suitable loading was anchored onto the external surface of a-SiO2, which could improve the dispersion of rodlike fibers of ATP. MEA loading and reaction temperature optimization experiments showed that the 50MEA/a-SiO2 sorbent achieved the highest CO2 adsorption capacity of 2.14 mmol/g with an amine efficiency of 5.22 mmol/g and 0.32 mol/mol at 60 °C. Furthermore, only a 6.3 and 4.7% reduction of CO2 adsorption capacity occurred after five adsorption–desorption cycles under simulated biogas at 30 and 60 °C adsorption, respectively, indicating that the sorbent has good regenerability and thermal stability. The chemical adsorption was proved to be the CO2 adsorption mechanism of MEA-modified ATP-based a-SiO2 sorbent by XRD and FTIR testing.

CAS / MDL: 67-56-1 142-58-5
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CERAMICS INTERNATIONAL · 2021 · IF 4.527

Li4SiO4 pellets templated by rice husk for cyclic CO2 capture: Insight into the modification mechanism

Yingchao Hu,Hongyuan Lu,Hailong Li

Li 4 SiO 4 stands out among various solid sorbents for CO 2 capture. The commonly used mechanical granulation process for Li 4 SiO 4 sorbents causes the destruction of the microstructures. Therefore, with the characteristics of huge production and low cost, an agricultural waste (rice husk) was employed as a pore former to improve the structures of Li 4 SiO 4 pellets and, thus, enhance the cyclic CO 2 sorption performance. The rice husk templating greatly enhanced the CO 2 sorption capacity of Li 4 SiO 4 pellets. Especially, 20 wt% rice husk-templated Li 4 SiO 4 exhibited the capacity of 0.21 g/g, which was nearly twice that of the unmodified sorbent. The quick release of the combustion gases from burning rice husk could create porosity for the sorbents. In addition, the alkaline compositions in rice husk promoted the CO 2 sorption due to the decreased CO 2 diffusion resistance by the formation of molten phases. Moreover, the ashes of rice husk after high-temperature combustion were found to block the pores of the sorbents, leading to the capacity reduction. The comprehensive function of rice husk templating for Li 4 SiO 4 pellets was the tradeoff between the positive effects of pore creation and alkaline doping and the negative effects of pore blockage by the ashes.

CAS / MDL: 546-89-4
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Enhanced stability and activity towards photocatalytic CO2 reduction via supercycle ALD of Cu and TiO2

Mu Liu,Xiaolei Bao,Fahao Ma,Minrui Wang,Liren Zheng,Zeyan Wang,Peng Wang,Yuanyuan Liu,Hefeng Cheng,Ying Dai,Yuchen Fan,Zhaoke Zheng,Baibiao Huang

Enhanced photocatalytic performance and excellent stability are usually regarded contradictory during photocatalytic reaction. In this study, supercycle ALD was employed to achieve superior performance and stability simultaneously for the system of TiO 2 @Cu during CO 2 reduction reaction, which was unattainable by post-deposition TiO 2 , a commonly-employed technique for enhancing stability. More oxygen vacancy, partially-covered Cu species as well as well-maintained charge separation capability of alternatively-deposited TiO 2 @(2Cu + 2TiO 2 ) × 25 could be the reason for enhanced activity and stability as suggested by a series of characterizations such as Single-particle TRPL and Single-particle PL. Experimental data also suggested unselective and mixed-layer deposition of TiO 2 and Cu loaded in the mode of alternative-deposition. The method proved in our study could be applicable in synthesizing other ALD-prepared catalysts with enhanced performance and stability, which will be a big step forward towards comprehensively utilizing the potential of ALD technique in the field of photocatalysis.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Veiled metal organic frameworks nanofillers for mixed matrix membranes with enhanced CO2/CH4 separation performance

Ke Chen,Linhan Ni,Hao Zhang,Jia Xie,Xin Yan,Saisai Chen,Junwen Qi,Chaohai Wang,Xiuyun Sun,Jiansheng Li

The interfacial compatibility between fillers and polymers essentially influences the separation performance of mixed matrix membranes (MMMs). In this work, an one-pot synthesized functional layer veiled zeolite imidazolate frameworks-67 (VZIF-67) was used as an efficient nanofillers to fabricate MMMs via physical blending with 6FDA-Durene polyimide. Benefiting from the CO 2 affinity from functional layer and the intrinsic characteristics of porous nanofillers, significant enhancement on separation performance was observed on the resultant MMMs. Specifically, the optimized VZIF-67 MMMs (30 wt% loading) exhibited CO 2 /CH 4 selectivity of 32.5 with CO 2 permeability of 1210 Barrer, which is 1.7 and 1.5 times higher than those of the control membrane, respectively. More importantly, the surface organic attribute and abundant amine groups of VZIF-67 reinforced the interfacial compatibility between the nanofillers and polymer matrix, leading to a doubled CO 2 /CH 4 selectivity compared with the ZIF-67 MMMs. Overall, the performance of the VZIF-67 membrane toward CO 2 /CH 4 separation surpasses the 2008-updated Robeson upper bound. These results indicate the functionalization strategy on porous nanofillers is a promising approach to fabrication of high performance of MMMs.

CAS / MDL: 1107-00-2 3102-87-2
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JOURNAL OF MOLECULAR LIQUIDS · 2021 · IF 6.165

Solubility of N2O and CO2 in nonaqueous blends of 2-(methylamino)ethanol and 2-methoxyethanol

Xiaoqin Shi,Shufeng Shen

Nonaqueous secondary alkanolamine-based systems, replacing conventional water with 2-alkoxyethanols as cosolvents, have recently attracted much attention for an energy-efficient CO 2 capture process. In this work, physical solubility of N 2 O and CO 2 in 2-(methylamino)ethanol (MAE), 2-methoxyethanol (2-ME) and their blends was measured and correlated at temperatures ranging from (283.2 to 333.2) K. Vapor-liquid equilibrium (VLE) data for the CO 2  + MAE + 2-ME system at 7.8, 19.4 and 39.1 mass% MAE were also measured in a stirred equilibrium cell at temperatures of (313.2–393.2) K and CO 2 partial pressures up to 270 kPa. VLE data were represented by a modified Kent-Eisenberg model with an AARD of 12.6%. The apparent equilibrium constants considering the liquid nonideality were well correlated as a function of temperature, concentration of carbamate product and CO 2 loading.

CAS / MDL: 109-86-4 109-83-1
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Sustainable Energy & Fuels · 2021 ·Vol. 5 ·期 17 ·4295-4310 · IF 6.367

Sr-doped SmMnO3 perovskites for high-performance near-isothermal solar thermochemical CO2-to-fuel conversion

Ke Gao,Xianglei Liu,Tong Wang,Zhonghui Zhu,Ping Li,Hangbin Zheng,Chao Song,Yimin Xuan,Yongliang Li,Yulong Ding

Solar thermochemical CO2-to-fuel conversion via two-step redox cycles is a promising strategy to solve climate change and energy storage challenges simultaneously. However, ideal thermochemical materials possessing moderate operation temperature, high yield, good stability, and rapid kinetics operating under isothermal and near-isothermal conditions are still missing. Here, we propose Sr-doped SmMnO3 for moderate-temperature near-isothermal CO2-to-fuel conversions. A record-high isothermal cycle CO yield (376.1 μmol g−1) at no more than 1300 °C is reported based on Sm0.6Sr0.4MnO3. No obvious decay is observed during 14 cycles although grain sizes have increased to some extent. The weakened Mn–O bond induced by Sr doping helps to create more oxygen vacancies, and thus contributes to enhanced yield of both O2 and CO. The oxidation reaction is fast with a CO yield of 58.6 μmol g−1 in 15 minutes, which is 5.6 times as high as that of CeO2 under the same cycling conditions between 1300 °C and 1000 °C. Detailed kinetics for the oxidation step is unveiled based on the Šesták–Berggren model. In addition, SmxSr1−xMnO3 can capture full-spectrum solar energy with a solar absorptance of more than 86.6% in stark contrast to 13.5% for CeO2, making the required concentration ratio to drive reactions decrease by 33.4%. This work provides new materials for high yield and stable thermochemical CO2-to-fuel conversion under moderate-temperature near-isothermal conditions, and paves the way for the development of CO2 splitting techniques directly driven by low-concentration solar energy with high efficiencies.

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Journal of Environmental Chemical Engineering · 2021 · IF 5.909

CO2 capturing and in situ conversion at mild condition: Efficient synthesis of methyl phenyl carbonate

Leizhi Zheng,Guoqiang Yang,Xingbang Hu,Zhibing Zhang

The capture and conversion of carbon dioxide (CO 2 ) into useful and valuable chemicals are receiving more and more research interesting. Herein, we designed a new and efficient route to synthesize methyl phenyl carbonate (MPC) via the carbonylation of phenol (PhOH) with CO 2 and methanol (CH 3 OH). PhOH and CH 3 OH react with 1,8-diazabicyclo-[5.4.0]undec-7-ene (DBU) to form ionic liquids [DBUH][PhO] and [DBUH][CH 3 O]. The DBU-based ionic liquids exhibited outstanding performance in CO 2 capture and in situ conversion at room temperature. The reusability of the system had no obviously change after 6 cycles. This protocol provides a sustainable and environmentally friendly preferential technique for the production of MPC, and extends the chemical utilization of CO 2 .

CAS / MDL: 67-56-1 108-95-2
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ACS Applied Nano Materials · 2021 · IF 5.097

SiO2-Coated Ag Nanoparticles for Conversion of Terminal Alkynes to Propolic Acids via CO2 Insertion

Minkang Li,Lina Zhang,Zhongzheng Zhang,Jialin Shi,Yuefeng Liu,Jiansong Chen,Nannan Sun,Wei Wei

Integration of adequate activity, stability, and productivity in a catalyst is of strategical importance to achieve high performance, particularly for inactive reactants, e.g., CO2. Here, using a reversed microemulsion method, ultrafine metallic Ag nanoparticles coated with porous SiO2 can be facilely obtained using micelles as separated nanoreactors for the preparation. Such architectures allowed the rigid SiO2 matrices to act as physical spacers, so that aggregation of the Ag particles could be avoided. Meanwhile, due to the templating effect from the surfactant, large mesopores could be induced in the SiO2 shell, and thus the diffusion barrier of reactants could be minimized. When used as a heterogeneous catalyst for carboxylation of terminal alkynes by CO2 under mild conditions, the prepared xAg@SiO2 catalysts showed extraordinary performance in terms of excellent activity, stability, productivity, and wide substrate scope. The knowledge developed here may also enrich the toolbox for performance promotion of metal catalysts via specially fabricated structures.

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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Bio-inspired design of strong self-standing cathode toward highly stable reversible Li-CO2 batteries

Xiao-Xue Wang,Gui-Juan Ji,Ping She,Fei Li,Qing-Chao Liu,Huan-Feng Wang,Ji-Jing Xu

The hysteresis kinetics of carbon dioxide reduction reaction (CDRR) and evolution reaction (CDER) reaction are major barriers toward the practical implementation of lithium-carbon dioxide (Li-CO 2 ) batteries. Herein, a free-standing and binder-free cathode composed of rutile TiO 2 nanorod arrays (TiO 2 NAs) and carbonized natural sponge was designed and realized by a simple seeds-assisted construction. The novel air cathode was found to exhibits a high specific capacity of 4.38 mAh cm −2 and long cycle life of more than 1600 h, as well as the discharge products, which would deposit at the surface of the TiO 2 NAs rather than carbon substrate during the discharge process. The improved performance can be ascribed to the interconnected conductive sponge framework with macropore and mesoporous channels that can house more discharge products, and the reactant molecules can unrestricted contact with the active sites. Furthermore, the good adhesion to the carbon substrate and the numerous available catalytic sites of the TiO 2 NAs contribute intimate contact of the discharge products with the TiO 2 NAs, improving CDRR and CDER kinetics effectively and boosting the electrochemical reactions. This TiO 2 /Sponge represents a promising design in the development of a nature-inspired, self-standing, and binder-free electrode for high-performance Li-CO 2 batteries.

CAS / MDL: 33454-82-9 143-24-8
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2021 · IF 19.503

A novel amorphous alloy photocatalyst (NiB/In2O3) composite for sunlight-induced CO2 hydrogenation to HCOOH

Jiehong He,Pin Lyu,Bo Jiang,Shaoshuai Chang,Haoran Du,Jian Zhu,Hexing Li

Photocatalytic CO 2 hydrogenation into fuels and value-added chemicals is considered as a promising strategy for CO 2 conversion and utilization. However, the photocatalysts used usually displays low efficiency and poor durability. Herein we developed a novel catalyst by combining NiB amorphous alloy with In 2 O 3 semiconductor, which exhibited very high HCOOH yield (5158.0 umol g −1 h −1 ) in CO 2 hydrogenation under sunlight irradiation. The In 2 O 3 acted as a photocatalyst for generating photoelectrons to reduce CO 2 and provided sufficient surface hydroxyl (In−OH) groups favouring CO 2 adsorption during the reaction. The high dispersion of NiB nanoparticles (co-catalyst) and interaction with In 2 O 3 provided the rich interface between NiB and In 2 O 3 , favoring the surface reactions between CO 2 and H 2 . Meanwhile, the unique amorphous alloy structure made the Ni electron-enriched, which promoted CO 2 hydrogenation through the H 2 dissociation. More importantly, the NiB amorphous alloy with good electric conductivity facilitated the transfer of photoelectrons from In 2 O 3 , which sufficiently diminished the photoelectron-hole recombination, leading to the enhanced quantum efficiency in photocatalytic CO 2 hydrogenation.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

CuBi electrocatalysts modulated to grow on derived copper foam for efficient CO2-to-formate conversion

Wenshuang Lou,Luwei Peng,Ruinan He,Yuyu Liu,Jinli Qiao

Electrochemical reduction of CO 2 to fuels and chemicals is an effective way to reduce greenhouse gas emissions and alleviate the energy crisis, but the highly active catalysts necessary for this reaction under mild conditions are still rare. In this work, we grew CuBi bimetallic catalysts on derived copper foam substrates by co-electrodeposition, and then investigated the correlation between co-electrodeposition potential and electrochemical performance in CO 2 -to-formate conversion. Results showed that the bimetallic catalyst formed at a low potential of − 0.6 V vs. AgCl/Ag electrode achieved the highest formate Faradaic efficiency (FE formate ) of 94.4% and a current density of 38.5 mA/cm 2 at a low potential of − 0.97 V vs. reversible hydrogen electrode (RHE). Moreover, a continuous-flow membrane electrode assembly reactor also enabled the catalyst to show better performance (a FE formate of 98.3% at 56.6 mA/cm 2 ) than a traditional H-type reaction cell. This work highlights the vital impact of co-electrodeposition potential on catalyst performance and provides a basis for the modulated growth of bimetallic catalysts on substrates. It also shows the possibility of preparing Bi-based catalysts with no obvious decrease in catalytic activity that have been partially replaced with more economic copper.

CAS / MDL: 141-53-7
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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Sawdust wastes-derived porous carbons for CO2 adsorption. Part 1. Optimization preparation via orthogonal experiment

Chen Jin,Jian Sun,Yuning Chen,Yafei Guo,Donghui Han,Ruilin Wang,Chuanwen Zhao

Sawdust wastes were used as the low-cost feedstock to prepare porous carbons by KOH activation, and the preparation parameters were optimized via orthogonal experiment. Four main activation parameters (i.e., sawdust type, KOH/sawdust ratio, activation temperature and activation time) were investigated. It is found that activation temperature and KOH/sawdust ratio are the two most important parameters that affect the porous texture properties (specific surface area and micropore volume) of sawdust wastes-derived porous carbons. The optimal sawdust wastes-derived porous carbon possesses a high specific surface area of 1601 m 2 /g and a micropore volume of 0.75 cm 3 /g, therefore exhibiting a desirable CO 2 adsorption capacity of 4.25 mmol/g at 0 °C under ambient pressure. Comparatively, the sawdust wastes-derived porous carbon extrudates exhibit the inferior CO 2 adsorption capacity, dropping to 2.85–3.03 mmol/g. It is mainly attributed to the extrusion treatment and binder addition causing the collapse and blockage of the original porous structure, consequently increasing the CO 2 diffusion and adsorption resistance. However, the sawdust wastes-derived porous carbon extrudates possess the advantages of null pressure build-up, improved bulk density and high compress strength (7.3–12.3 MPa) considering the real application point of view.

CAS / MDL: 1310-58-3
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