CHEMICAL ENGINEERING SCIENCE
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2022
·
IF 4.889
Qinlan Luo,Qiang Sun,Qi Liu,Sen Liu,Min Xiao,Mengjie Chen,Yuanyuan Li,Hongxia Gao,Zhiwu Liang
The kinetics of CO 2 absorption in ethanolamine (MEA) + H 2 O + ethanol systems was investigated using stopped-flow apparatus. The first-order reaction rate constant ( k 0 ) values were tested with varying H 2 O and MEA concentrations. Transiting from the aqueous to non-aqueous solvents, the k 0 decreases and the reaction order for MEA shifts from 1.05 to 1.88. The zwitterion mechanism with the rate-limiting step of deprotonation was used to explore the role of water and its effect. Results showed that water could impact reactions through direct involvement and changing solvation environment. An improved kinetic model based on the zwitterion mechanism was obtained to indicate the quantitative influence of H 2 O concentration on the reaction kinetics of MEA + H 2 O + ethanol systems. The predicted values from the model well agreed to the experimental data with the average absolute relative difference of 6.73%. This study highlights the important effects of water on the reaction kinetics of CO 2 absorption into water-lean amine solutions.
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JOURNAL OF MEMBRANE SCIENCE
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2022
·
IF 10.53
Jinyin Lv,Xuerong Zhou,Jianhua Yang,Lei Wang,Jinming Lu,Gaohong He,Yingchao Dong
A well-intergrown and defect-free tubular KAUST-7 membrane was fabricated via in-situ synthesis assisted by fluorinated molecular building block using green solvent of water on coarse asymmetric α-Al 2 O 3 tubes. The strategy averted the serious corrosion of high-concentration hydrofluoric acid (HF) to α-Al 2 O 3 supports due to the substitution of HF with the pre-synthesized NiNbOF 5 , overcoming the difficulty of serious corrosion to supports compared to traditional one-pot synthesis. The pH manipulation of synthesis solution is proved crucial to the fabrication of defect-free KAUST-7 membranes. In addition, effects of reactant concentration, crystallization temperature and reaction solvents on the morphology and separation performance of KAUST-7 membrane were investigated. The optimized KAUST-7 membrane M4 exhibited a H 2 perm-selectivity of 17.7 over CO 2 for H 2 /CO 2 binary mixture with a H 2 permeance of 2.2 × 10 −7 mol m −2 s −1 Pa −1 at 25 °C and 1 bar, while the H 2 /CO 2 separation factor just had a slight decrease when test temperature increased to 120 °C. The formation mechanism of KAUST-7 membranes via in-situ method in this work was investigated by exposing a bare α-Al 2 O 3 tube into NiNbOF 5 aqueous solution at the pH of 4.0 at 130 °C for 12 h. XPS and FT-IR observations revealed the formation of AlF x O y or AlF x species, which were deduced to be acted as linkers to connect with 2D Ni (II)-pyrazine layers, promoting the heterogeneous nucleation of KAUST-7 crystals on the surface of Al 2 O 3 support.
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POLYMER
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2022
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IF 4.432
Hongzhou Xie,Hongxu Meng,Linbo Wu,Bo-Geng Li,Philippe Dubois
Poly(ethylene 2,5-furandicarboxylate) (PEF) is a promising biobased polymer possessing high strength , rigidity and gas barrier performance, but its poor ductility and toughness may limit its practical applications. In order to obtain PEF materials with improved ductility and impact toughness as well as high strength, modulus and excellent gas barrier performance, PEF with relatively low molecular weight was modified with aliphatic polycarbonate (APC) diols by chain extension/coupling in this study. The resulting products were mixtures composed of randomly segmented copolymers , chain extended APC and chain extended PEF. The APC moiety was proved to be partially miscible with the PEF matrix, and therefore plasticized the PEF matrix and promoted its cold crystallization. In comparison with PEF, the modified PEFs possess significantly enhanced tensile ductility and impact toughness. Particularly, the modified PEF containing 15 wt% poly(hexamethylene carbonate) exhibits balanced mechanical properties and CO 2 barrier 5 times to PET .
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 20
·8036-8045
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IF 4.569
Shengqi Xu,Lu Yang,Yixuan Wei,Yiming Jia,Meiqi Hu,Lianxia Bai,Junzheng Zhang,Xinxin Li,Shuo Wei,Jun Lu
Converting CO2 into valuable solar fuels through photocatalysis has been considered a green and sustainable technology that is promising for alleviating global warming and providing energy in an environmentally friendly manner. However, traditional photocatalysts generally suffer from low surface-reactive reaction sites, inefficient light harvesting and rapid recombination of electron–hole pairs. Lead halide perovskite materials have been considered ideal semiconductor photocatalysts for photocatalytic CO2 reduction due to their tunable band gaps, strong light absorption, and low cost. Herein, a series of L2Csn−1PbnX3n+1 (L = ba, ha, oa; X = Cl, Br, I; n = 1, 2) 2D layered perovskites were synthesized by a facile solvothermal method. The effects of alkyl amine chain length, halogen atoms and inorganic layer number on their properties were studied. More importantly, these 2D materials were used as photocatalysts for CO2 reduction without any sacrificial agents. These 2D perovskites exhibited markedly increased performance in comparison with 3D bulk materials, benefitting from the larger surface-area-to-volume ratio and faster and more efficient exciton dissociation, which achieved the highest CO yield of 158.69 μmol g−1 h−1 and CH4 yield of 6.9 μmol g−1 h−1 through the design of the photocatalytic system. In addition, the influence of light source conditions on photocatalysis was studied systematically, including light source intensity and wavelength. The experimental results indicated that an appropriate solvent, high light intensity and monochromatic light source matching the wavelength of exciton absorption can effectively improve the photocatalytic efficiency.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
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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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
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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JOURNAL OF APPLIED POLYMER SCIENCE
·
2022
·Vol. 139
·期 30
·e52661
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IF 3.057
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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ELECTROANALYSIS
·
2022
·Vol. 35
·期 1
·e202200158
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IF 3.077
Liangyin Zhou,Hongji Li,Dandan Wang,Wei Jiang,Yuanyuan Wu,Liaofang Shang,Chunyi Guo,Chunbo Liu,Baixiang Ren
Zeolitic Imidazolate Frameworks (ZIFs) are considered as a novel porous material combining high stability in inorganic zeolites with high porosity and organic functionality of MOFs. The cage-like structure selectively and efficiently traps CO 2 , which is an indispensable and critical step for Electrocatalytic CO 2 Reduction Reaction (CO 2 RR). In this work, ultrasmall ZIF-8 nanomaterials are synthesized by tuning the molar ratio of the feedstock and used as electrocatalysts for the selective reduction of CO 2 to CO. The catalytic activity of the ultra-small size ZIF-8 material for the electrocatalytic reduction of CO 2 can reach satisfactory results with a Faraday efficiency of 91 % for CO and a stability of 12.5 h at a high applied potential of −1.8 V vs. RHE. The investigation can provide a new idea to explore for the design and improvement of catalysts for CO 2 RR.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2022
·
IF 6.76
Liwei Sun,Meilin Yin,Zhen Li,Shaokun Tang
To alleviate environment issues derived from CO 2 emission, developing effective and economical methods for CO 2 capture has attracted much attention for decades. Metal-organic frameworks possess high porosity and stability, which is favorable to the adsorption of small molecules. Herein, an aluminum-based MOF, aluminum terephthalate [MIL-53(Al)], was synthesized with H 2 O and N , N′ -dimethylformamide as co-solvent via microwave-assisted method for CO 2 adsorption. The parameters including pre-mixing mode, microwave temperature, microwave power and reaction time were varied to study their influences on crystal structure, morphology and CO 2 adsorption capacity of MW-MIL-53(Al). Wherein, MW-MIL-53(Al) prepared with pre-mixing mode of stirring at 130 °C, 200 W and 3 h presents high crystallinity and rod-like morphology. The synthesized MW-MIL-53(Al) possesses relatively high BET surface area (961 m 2 /g), pore volume (0.46 cm 3 /g) and thermal stability (up to 480 °C), and its CO 2 adsorption capacity is 2.16 mmol CO 2 /g adsorbent under 25 °C and 0.1 MPa, which is higher than CS-MIL-53(Al) synthesized via conventional solvothermal method at 130 °C for 48 h.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2022
·Vol. 139
·期 27
·e52485
·
IF 3.057
Xiaoshuai Zhu,Xijue Li,Hao-Yang Mi,Xin Jing,Binbin Dong,Ping He,Chuntai Liu,Changyu Shen
Thermoplastic polyurethane (TPU) foams are commonly used buffering materials due to their lightweight, high elasticity, and excellent energy absorption properties. Improving their compressive property without increase foam density is a challenge for TPU foams. Herein, graphene oxide (GO)/TPU composite foams containing micro-sized wrinkles on the cell surface were fabricated by a novel dynamic supercritical carbon dioxide (scCO 2 ) foaming method. The addition of GO created hydrogen bonding and physical crosslinking sites with the TPU molecules, which acted as nucleation agents to improve the cell density of the GO/TPU foams. With the increase of GO content, the mechanical properties of GO/TPU foams were significantly enhanced, and the wrinkled foams prepared via dynamic scCO 2 foaming displayed superior compressive modulus, strength, energy absorption, and recoverability compared with the counterpart foams without wrinkly structure. The wrinkled GO/TPU foams with 0.5 wt% GO revealed higher expansion ratio, lower foam density, superior compressive property and energy absorption than both neat TPU and 1 wt% GO foams owing to the reinforcing effect of the wrinkly structure. This study is of great significance in the development of low-density composite foams with enhanced compressive performance by wrinkly structures.
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ChemSusChem
·
2022
·Vol. 15
·期 14
·e202200337
·
IF 9.14
Li-Qi Qiu,Zhi-Wen Yang,Xiangyang Yao,Xiao-Yang Li,Liang-Nian He
Graphical CO 2 photoreduction : Toward building robust artificial photosynthetic systems, a series of single-active-site rhenium bipyridyl complexes with dipyrromethene-BF 2 units exhibit outstanding catalytic efficiency for visible light-driven-CO 2 reduction. New rhenium bipyridyl complexes with dipyrromethene-BF 2 chromophores (A-ReBDP-CZ, A-ReBDP 2 , ReBDP-CZ, and ReBDP 2 ) were developed for highly efficient photocatalytic carbon dioxide (CO 2 ) reduction to carbon monoxide (CO). These catalysts consisted of two moderate electron-deficient groups (dipyrromethene-BF 2 , BDP) as the visible-light-harvesting antenna as well as both electron donor ( N -phenylcarbazole, CZ) and acceptor (BDP) on Re bipyridyl framework. Among ReBDP-CZ and ReBDP 2 complexes, the ReBDP 2 incorporating two electron-deficient BDP chromophores had a longer-lived photoexcited state (182.4 μs) and a twofold enhanced molar absorption coefficient ( ϵ =157000 m −1 cm −1 ) compared with ReBDP-CZ. Thus, ReBDP 2 achieved the superior photocatalytic reactivity and stability with a CO turnover number (TON CO ) value as high as 1323 and quantum yield ( Φ CO ) up to 55 %, which was the most excellent photocatalysis efficiency among the single-active-site Re catalysts without additional photosensitizer. Furthermore, the acetylene-bridged linker was detrimental to the photoactivity and durability of the catalyst. In brief, two BDP-based Re bipyridyl systems with outstanding catalytic performance and significant visible-light-harvesting capabilities in the solar spectrum offer a promising strategy for solar-to-fuel conversion schemes.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
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.
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