ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Yakun Sun,Long Li,Xinxu Li,Ya-Nan Feng,Fei-Fei Chen,Lingyun Li,Yan Yu
Cobalt-based catalysts are ideal for CO2 reduction reaction (CO2RR) due to the strong binding and efficient activation of CO2 molecules on cobalt. However, cobalt-based catalysts also show low free energy of hydrogen evolution reaction (HER), making HER competitive with CO2RR. Therefore, how to improve the product selectivity of CO2RR while maintaining the catalytic efficiency is a great challenge. Here, this work demonstrates the critical roles of the rare earth (RE) compounds (Er2O3 and ErF3) in regulating the activity and selectivity of CO2RR on cobalt. It is found that the RE compounds not only promote charge transfer but also mediate the reaction paths of CO2RR and HER. Density functional theory calculations verify that the RE compounds lower the energy barrier of *CO → CO conversion. On the other hand, the RE compounds increase the free energy of HER, which leads to the suppression of HER. As a result, the RE compounds (Er2O3 and ErF3) improve the CO selectivity of cobalt from 48.8 to 69.6%, as well as significantly increase the turnover number by a factor of over 10.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jian Wang,Yan Zhang,Jiwen Si,Wei Zhang,Qing Liang,Wenqing Li,Bo Jin,Shiding Miao
The cost- and use-effects for solid CO 2 adsorbents have accelerated development of the clay-based adsorbents. Herein, a series of NiFe-layered double hydroxides/halloysite (NiFe-LDH/Hal) composites were fabricated via facile hydrothermal strategy using calcined halloysites (Hal) as supports. Depending on treatment temperatures of halloysite, the supported NiFe-LDH exhibited different morphologies in form of nanoparticle or intertwined nanosheets. Based on the distinct morphology, these NiFe-LDH/halloysite composites displayed different textural properties and CO 2 adsorption performance. Particularly, the sample NiFe-LDH/Hal600 using halloysite calcined at 600 °C as support possessed 3D hierarchical structure, and displayed superior CO 2 adsorption capacity of 60.7 mg g −1 and 40.3 mg g −1 at 273 K and 298 K, respectively, much higher than those of NiFe-LDH/Hal composites supporting LDH nanoparticles. The high isosteric heat of adsorption calculated from Clausius-Clapeyron equation (21.7 kJ mol −1 ) indicated the strong interaction between basic NiFe-LDH surface and CO 2 molecules. It was validated that the dehydroxylation and forming of silanols groups during calcination process changed the activity of internal and external surface, resulting in distinct morphology and distribution difference of the supported NiFe-LDH. The prepared clay-based composites displayed satisfying recyclability of CO 2 adsorption at a high retention level after 25 cycles of adsorption–desorption.
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Catalysts
·
2023
·Vol. 13
·期 3
·600
·
IF 3.9
Jiajia Wei,Xing Chen,Xitong Ren,Shufang Tian,Feng Bai
Due to the different electron affinity, the construction of a donor-acceptor (DA) system in the graphitic carbon nitride (g-CN) matrix is an attractive tactic to accelerate photo-induced electron-holes separation, and then further elevate its photocatalytic performance. In this work, perylene tetracarboxylic dianhydride (PTCDA) with magnificent electron affinity and excellent thermal stability was chosen to copolymerize with urea via facile one-pot thermal copolymerization to fabricate g-CN-PTCDA equipped with DA structures. The specific surface area of g-CN-PTCDA would be enlarged and the visible light absorption range would be broadened simultaneously when adopting this copolymerization strategy. A series of characterizations such as electron paramagnetic resonance (EPR), steady and transient photoluminescence spectra (PL), electrochemical impedance spectroscopy (EIS), and photocurrent tests combined with computational simulation confirmed the charge separation and transfer efficiency dramatically improved due to the DA structures construction. When 0.25% wt PTCDA was introduced, the CO evolution rate was nearly 23 times than that of pristine g-CN. The CO evolution rate could reach up to 87.2 μmol g−1h−1when certain Co2+was added as co-catalytic centers. Meanwhile, g-CN-1 mg PTCDA-Co exhibited excellent long-term stability and recyclability as a heterogeneous photocatalyst. This research may shed light on designing more effective DA structures for solar-to-energy conversion by CO2reduction.Keywords:donor-acceptor;graphitic carbon nitride;PTCDA;photocatalysis;CO2reduction
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yongchao Sun,Jingfa Zhang,Hongjin Li,Fangxu Fan,Qizheng Zhao,Gaohong He,Canghai Ma
Polymers of intrinsic microporosity (PIMs) have seen a growing role in gas separation membranes. Further exploitation of gas separation performance of PIM membranes and overcoming their persistent challenge of plasticization are urgently demanded. To address these issues, exemplified PIM-1 is synthesized and hydrolyzed to form carboxylated PIM-COOH polymers, followed by esterification using propylene glycol to prepare monoesterified PIM, which is finally thermally ester-crosslinked at various temperatures and time. The 300 °C-8 h treated membranes exhibit a CO 2 permeability of 7421 Barrer, with a CO 2 /CH 4 and CO 2 /N 2 selectivity of 11.5 and 19.2, respectively, considerably exceeding the 2008 Robeson upper bounds. Furthermore, the crosslinked membranes demonstrate significantly enhanced CO 2 plasticization resistance up to 42 bar, compared with uncrosslinked ones. It is the first time of reporting ester-crosslinking of carboxylated PIM-1 with both higher gas permeability and selectivity than PIM-1, using a much milder crosslinking temperature than other techniques, such as decarboxylated crosslinking. The design principle of this work paves the way for preparing high-performance and plasticization-resistant PIM membranes with promises for energy-efficient gas separations.
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Materials Today Nano
·
2023
·
IF 10.3
L.K. Pan,J.C. Qi,H. Mei,L. Yao,H.X. Liu,S.X. Zhou,G.Q. Zhu,J.J. Wang,L.F. Cheng,L.T. Zhang
Developing efficient and highly selective photocatalytic CO 2 reduction catalysts remains one of the most significant challenges in achieving carbon neutrality . Herein, the efficient conversion of CO 2 to CH 4 with selectivity close to 100% was achieved by loading uniformly dispersed Pt nanoparticles on the surface of Sr 2 Nb 2 O 7 nanosheets ; the optimal CH 4 yield was as high as 15.65 μmol/g/h. Various characterizations demonstrate that Pt nanoparticles have a significant photothermal effect that can increase the catalyst surface temperature, and improve the performance and electron transport rate of the catalyst. Additionally, Pt nanoparticles and Sr 2 Nb 2 O 7 nanosheets form heterojunctions , which facilitate the separation of photogenerated carriers and aggregation of photogenerated electrons on the Pt nanoparticles. Pt nanoparticles become new reactive sites that have a strong adsorption impact on the key intermediate ∗CO and reduce the reaction energy barrier of ∗CHO generation. The results revealed that the synergy between electron accumulation, strong adsorption of ∗CO, and reduction of the reaction potential of ∗CHO are the reasons for the efficient and selective conversion of CO 2 to CH 4 . This work provides novel insights into the role of metal-based cocatalysts in selective CO 2 photoconversion and new ideas for designing efficient CO 2 conversion systems.
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POLYMER
·
2023
·
IF 4.6
Ke Wang,Liru An,Ganghui Lu,Jialu Zhang,Zilong Wang,Meiyu Si,Guiyan Liu,Yongfei Zeng
A series of novel thermo/pH/CO 2 -triple responsive homopolymers were synthesized by reversible addition-fragmentation chain transfer (RAFT) polymerization. These homopolymers contain ethoxy groups , and the end substituents are pyrrolidine , piperidine , N -methylpiperazine, morpholine and thiomorpholine , respectively. The effects of different heterocyclic substituents on the responsiveness of temperature, pH and CO 2 were studied. For temperature-response, it was found that the lower critical solution temperature (LCST)-type cloud point (CP) temperature decreased as the number of carbon atoms increases, while the solubility of the polymers changed greatly with the introduction of oxygen, nitrogen and sulfur atoms. And the CP of the polymers can be adjusted by molecular weight , concentration and salt. Furthermore, some of these polymers present upper critical solution temperature (UCST) behavior in alcohols. For pH-response, the initial pH of the polymer solution is different, their critical pH changed accordingly, and is affected by temperature; in addition, changing the pH of solution can also affect the CP. For CO 2 -response, all of the polymers were completely soluble after pumping with CO 2 , and their LCST behavior recovered after N 2 was pumped in, but there was a gap with the initial CP. The study of these properties reveals the influence of different heterocyclic substituents on the responsiveness of polymers, which is of great significance for understanding the stimulation response properties of polymers and provides ideas for the design of new stimuli-responsive polymers.
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JOURNAL OF POLYMER SCIENCE
·
2023
·Vol. 61
·期 17
·2025-2036
·
IF 3.4
Tao Li,Zhijian Liu,Yao Chen,Na Sun,Haozhou Shu,Lili Wu,Chaocan Zhang,Dong Xie
Two-component catalysts composed of tetra ( para -X substituted) phenylporphyrin aluminum (III) chloride, T ( p -X-P)PAlCl, (where X = H, F, Cl, Br, CH 3 , OCH 3 , tert -butyl), and cocatalyst bis(triphenylphosphine)imminium chloride (PPN + Cl − ), could initiate the polymerization of propylene oxide (PO). And they could react with rac -lactide, ( rac -LA), in the presence of propylene oxide (PO), to yield chains of enriched isotactic polylactide (PLA) with trace polyether segment. Also, these catalysts displayed different catalytic activity in the copolymerization of CO 2 and PO, resulting in poly(carbonate-co-ether) copolymer with different carbonate unit content (CU%). Further, these catalysts could initiate one-pot regio- and stereo- selective terpolymerization of rac -LA, CO 2 and rac -PO, resulting in multi-blocky poly(carbonate-co-lactide) with trace polyether segment. The structure of the products was verified by 1 H NMR, 13 C NMR, GPC, and DSC analysis, and it was found that variation of substitution groups in the periphery of porphyrin ligand would affect on the catalytic efficiency of ter-polymerization, and the relative polymerization reaction ratio of the ring-opening polymerization of LA (ROP) to the ring-opening copolymerization of PO and CO 2 (ROCOP), resulting in ter-polymer with different contents of PLA segment and PPC segment. However, H-T % in polycarbonate unit and P i % in polylactide unit did not vary much with the change of catalysts. Graphical
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Journal of CO2 Utilization
·
2023
·
IF 7.7
Qin Fang,Huanda Zheng,Shengnan Li,Tao Cai,Fuer Zheng,Laijiu Zheng
Large degree of orientation, crystallinity, and high glass transition temperature of aramid make the fibers exhibit ultra-high strength, high modulus, high temperature resistance, acid and alkali resistance, light weight and other excellent properties. However, the resulting poor dyeability and water pollution problems of aramid greatly limits its application in protective areas. An eco-friendly supercritical CO 2 assisted printing strategy for meta-aramid was developed firstly in this study. The effects of treatment temperature, time, pressure and dye concentration on the printing properties were investigated. The obtained results showed that the K/S values of the printed meta-aramid increased with the enhancing of CO 2 temperature, treatment time and CO 2 pressure. Compared to tradition printing, higher color depth can be obtained by supercritical CO 2 assisted printing with 40% sodium carboxymethyl cellulose and 20% guar gum as original paste. The K/S values of the meta-aramid with Cationic Pink X-FG in supercritical CO 2 was 12.18 while that of the samples with Cationic Yellow 5GL was 5.42. Washing and rubbing colorfastness rated above 4 were reached at 180 °C for Cationic Pink X-FG and at 160 °C for Cationic Yellow 5GL in supercritical CO 2 . In addition, up to 99% outline sharpness and acceptable stiffness, air permeability and mechanical properties was obtained, which demonstrated that the meta-aramid fabrics with supercritical assisted printing could better meet the wearability requirements.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2023
·
IF 3.8
Wenjian Yue,Xiaojiang Li,Junhao Jing,Li Tong,Na Wang,Hongsheng Lu,Zhiyu Huang
Dining lampblack as a source of atmospheric pollution, urban residents had to spend a lot of economic costs all year round to solve its impact. However, traditional treatment methods often carry the risk of secondary pollution. The use of phase change absorption solvent (PCAS) controlled by CO 2 can effectively absorb the oily components in dining lampblack, and smoothly avoid the generation of secondary pollutants and squandering of resources. The reversibility of PCASs under CO 2 control was explained by pH changes and macroscopic visualizations. The absorption effects of favorable absorbents and PCASs on dining lampblack were compared and analyzed. The fatty acid (FA) in the oil absorption mixture was desorbed by interacting with D230. The results of GC/MS analysis on the oil components separated by desorption showed that the desorption of PCASs was effective for these refractory oil components. FAs can be enriched and applied to the subsequent dining lampblack treatment link to realize the waste recycling. In addition, the absorption and desorption of oily components by PCASs were combined with the CO 2 -controlled phase transformation of PCASs itself to achieve the absorption circulation of treating dining lampblack by using PCASs.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Huangying Wang,Haiyang Yan,Kang Peng,Junying Yan,Rong Fu,Ruirui Li,Baoying Wang,Chenxiao Jiang,Yaoming Wang,Tongwen Xu
The growth of CO 2 emissions is a critical challenge to the global ecological system. Meanwhile, the rising use of evaporation units in industrial wastewater treatment plants has generated a large number of salts with low values for further valorization. In this study, a direct electrochemical substitution electrodialytic system is proposed for the conversion of CO 2 and Na 2 SO 4 into high value-added NaHCO 3 and H 2 SO 4 . The CO 2 is absorbed with polyethyleneimine and further metathesized with inorganic salts in an electrodialytic reactor. This unique system achieves soda preparation by avoiding the use of ammonia as a feedstock and demonstrates the ability to capture and convert CO 2 at a specific energy consumption of 1.2 kWh/kg NaHCO 3 and a current efficiency of 83%. This proof-of-concept study provides a highly effective technological pathway for the conversion of notorious wastes into valuable resources, creating possibilities for concurrent carbon reduction and wasted salt utilization.
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Molecular Catalysis
·
2023
·
IF 4.6
Junqiang Li,Weifeng Huang,Zhuoyue Wang,Xiao Xu,Miao Sun,Longtian Kang
The carbon-based materials with metal-N-C active sites have been widely studied on the electrocatalysis for carbon dioxide reduction reaction (CO 2 RR), however, they were investigated a few for the photocatalytic CO 2 RR. Here, cobalt phthalocyanine (CoPc) molecules with intrinsic Co-N 4 -C moiety are successfully dispersed on graphene oxide (GO) as the CO 2 RR photocatalyst. The morphology, structure, and component of CoPc/GO composites with the different ratio of GO to CoPc are systematically characterized, confirming the existence of Co-O-C axial coordination bond between CoPc and GO. The optical, photoelectric, and electrical properties of CoPc/GO composites are carefully investigated, indicating their synergistic role of CoPc and GO in photocatalysis. With the optimal CoPc/GO sample as photocatalyst, a ∼1500 μmol⋅g − 1 ⋅h − 1 evolution rate and ∼ 85% selectivity of CO and CH 4 can be achieved, which is much higher than those performances of CoPc. After the reduction of CoPc/GO to CoPc/rGO, the rate of CO 2 RR to CO and CH 4 is reduced to 916 μmol⋅g − 1 ⋅h − 1 , indicating the important role of Co-O-C axial bond in the CO 2 RR. This work provides a simple way to prepare the single-molecule catalyst for CO 2 RR.
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RARE METALS
·
2023
·Vol. 42
·期 7
·2284-2293
·
IF 8.8
Du Juan,Lin Qin-Yan,Zhang Jian-Qi,Hou Sen-Lin,Chen Ai-Bing
Herein, we successfully prepare highly dispersed and uniform small nano-size nickel nanoparticles embedded on core–shell carbon spheres by confined-deposition method. The mesoporous silica layer containing surfactant coated on the surface of the polymer sphere provides confined space and effectively controls the growth of nickel nanoparticles during pyrolysis. At the same time, the introduction of nickel species has an impact on structure of the obtained carbon spheres, and it can promote the deposition of carbon to realize the adjustment from hollow to core–shell and then to solid spheres. Owing to the uniform distribution of Ni nanoparticles with small size, mesoporous structure, N-doping groups, high specified surface areas, and core–shell structure, the obtained catalyst shows exciting ability for the production of CO by reduction of CO 2 with a maximum CO Faradaic efficiency of 98%, indicating its promising prospect in electro-reduction of CO 2 . Graphical Abstract
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