CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Wenlu Luo,Wei Lu,Qin Xiang,Lianlong Zhan,Xun Yang,Hanbing Jiang,Cailin Xu,Hui He
The utilization of the solar-driven CO 2 desorption of carbon capture materials opens a promising avenue to reduce energy consumption in the carbon capture process. A crucial aspect is the careful coordination of materials' adsorption capacity and regeneration temperature. In this study, a photothermal responsive carbon capture material was developed by incorporating a photothermal responsive cellulose nanofiber matrix skeleton with a temperature-sensitive Pluronic® F-127 and polyethyleneimine. These components formed a staggered network through crosslinking with epichlorohydrin. The devised preparation strategy demonstrated a remarkable conversion rate of 99% for the reaction reagents. The resulting carbon capture material exhibited a high amino density of 14.18 mmol/g and a substantial adsorption capacity of 6.92 mmol/g. Notably, the shrinkage of Pluronic® F-127 molecular chains at elevated temperatures led to an increased surface electrostatic potential and the passivation of amino groups. This transformation endowed the material with a solar-driven regeneration temperature as low as 55 °C, representing an efficient approach to reduce energy consumption during the regeneration process of carbon capture materials.
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JOURNAL OF CATALYSIS
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2025
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IF 6.5
Jia Li,Yang Li,Yingshan Zeng,Yang Liu,Zhengguo Song,Zhi Liu
CO 2 photo reduction provides a feasible technique to solve climate issues and promote carbon neutrality. However, the efficiency of CO 2 photo reduction is severely depressed by the rapid recombination of photo generated carriers within photo catalysts, restricting the participation of electrons in the reduction process. In this study, we successfully construct a two-dimensional (2D) multilayer internal electric field (IEF) heterostructure by engineering the interface between NiAl-LDH and ZnV 2 O 6 (ZNA). Driven by the IEF, the separation of photo generated electron-hole pairs is significantly enhanced, leading to the increased utilization efficiency of carriers for active sites. The best-performing sample of ZNA-2 achieves a highest CO yield of 695.8 μmol g −1 , approximately 30.5-fold higher than that of pristine ZnV 2 O 6 . Photo electrochemical measurement and density functional theory (DFT) calculation results reveal that the 2D-2D stacked structure generates multiple interlayer built-in electric fields, which are crucial for enhancing carrier separation and suppressing recombination. Adsorption energy and intermediate COOH* analysis reveal that ZNA-2 significantly lowers the adsorption energy of CO 2 , promoting its stable adsorption and subsequent conversion. Moreover, the unique 2D multilayer IEF heterostructure greatly facilitates the formation of key intermediate COOH* and the desorption of CO during CO 2 photo reduction, leading to high CO activity and selectivity. The present work discloses the unprecedented potential of 2D multilayer IEF heterostructures for efficient CO 2 photo reduction, marking a significant advancement over conventional 2D counterparts.
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Chem
·
2024
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IF 19.1
Yaolin Wang,Jiaqiang Yang,Yuhai Sun,Daiqi Ye,Bin Shan,Shik Chi Edman Tsang,Xin Tu
Plasma catalysis offers a flexible and decentralized solution for CO 2 hydrogenation to methanol under ambient conditions, avoiding the high temperatures and pressures required for thermal catalysis. However, the reaction mechanism, particularly plasma-assisted surface reactions, remains unclear, limiting the development of efficient catalysts for selective methanol synthesis. Here, we report a bimetallic Ni-Co catalyst effective in plasma-catalytic CO 2 hydrogenation to methanol at 35°C and 0.1 MPa, achieving 46% methanol selectivity and 24% CO 2 conversion. In situ plasma-coupled Fourier transform infrared characterization, along with density functional theory calculations, reveals that the engineered bimetallic sites act as primary active centers for methanol synthesis, promoting the rate-determining step in H-radical-induced reaction pathways by reducing steric hindrance effects. This work demonstrates the significant potential of bimetallic catalysts in plasma-catalytic CO 2 hydrogenation to methanol under ambient conditions, representing a major step toward sustainable CO 2 conversion and fuel production.
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ACS Sustainable Chemistry & Engineering
·
2024
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IF 7.1
Jiasheng Tong,Miao Wang,Xuejun Qiu,Shizhen Li,Hangqi Yang,Chuang Peng
Deep eutectic solvents (DESs) are promising media for CO2 electroreduction because of their high CO2 solubility, low cost, and eco-friendliness. However, the high viscosity and poor ionic conductivity severely limit their applications. In this study, low-viscosity polar aprotic solvents, propylene carbonate (PC) and sulfolane (SL), were used as diluents in Ethaline (ChCl:2EG) to prepare mixed electrolytes for electrochemical CO2 reduction. Raman and infrared spectra indicate that PC and SL can participate in the eutectic network of Ethaline through intermolecular hydrogen bonding, thereby decreasing the viscosity. The current density of the Ag cathode increases from 1.7 to 8.0 and 5.3 mA/cm2 with the addition of PC and SL, respectively. The two diluents also result in improved CO faradaic efficiency (FECO) and suppressed HER because the C═O and S═O bonds in the molecular frameworks of PC and SL can disrupt the hydrogen bonds of accumulated water molecules during electrolysis. At −2.0 V, FECO increases from 63% to over 90% upon the addition of PC and SL. This study provides new insights into the design of high-performance DES electrolytes for CO2 electroreduction.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Rui Zhai,Zhenyu Wang,Mengyue Gu,Haoliang Liu,Xuewen Zhao,Jiangfan Li,Yaqiong Su,Yonghong Cheng,Shaobin Wang,Jinying Zhang
Selective photoreduction of CO 2 into ethylene is desirable but stays challenging due to easy desorption of primary reduction product CO. Herein, violet phosphorene nanosheets (VPNS) are for the first time demonstrated to be effective CO 2 photoreduction catalysts to yield ethylene. Photoelectron was found to transfer from VPNS to co-catalyst Ag and aggregated on VPNS-Ag interface to enhance CO 2 and CO* adsorption, and further lower the reduction energy barrier to yield ethylene, which was confirmed by in-situ diffuse reflectance infrared Fourier-transform, CO stripping voltammetry, CO reduction experiments, and density functional theory calculations. CO 2 is reduced into COOH* and automatically transformed into CO* on VPNS-Ag surface, then protonized into CHO* with a low barrier of 0.64 eV and automatically coupled into COCHO* to yield ethylene. Only ethylene was detected from CO 2 photoreduction with a yield of 10.34 μmol g −1 h −1 without any hole-sacrificial agent, much higher than most reported photocatalysts.
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Chemical Engineering and Processing-Process Intensification
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2025
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IF 3.9
Meng-Meng Du,Yuan-Cheng Wang,Bao-Chang Sun,Yong Luo,Liang-Liang Zhang,Guang-Wen Chu,Hai-Kui Zou
Carbonic anhydrase (CA) is a high-efficiency biocatalyst that significantly improves the absorption of CO 2 by tertiary amine. This work aims to investigate kinetics behaviors from the perspective of enzymatic reaction mechanism. The influences of the CA concentration, type of tertiary amines, pH, and temperature on the reaction rate between CO 2 and tertiary amine ( ν ) and catalytic activity of CA ( φ ) were first investigated in a stopped-flow device. Adding 50 g∙m⁻³ CA enhanced ν in tertiary amine solutions by a factor ranging from 22 to 42 at 298 K and pH=9.5, demonstrating its excellent catalytic performance. The ν increased with increasing CA concentration, pH, temperature, and tertiary amine's pK a. φ increased with the increase of CA concentration, as well as the decrease of temperature, pH, and tertiary amine's pK a. Proteomics analysis further revealed that conformational changes of the CA's secondary structure induced by high pH and temperature altered the expressions of the local active-site region and deactivated CA, ultimately leading to a decrease in φ . Additionally, the CA-catalysis kinetics equation accorded with the Michaelis-Menten model, with catalytic second-order rate constants on the magnitude of 10 7 . Overall, this work provides a guideline for its industrial application in the CO 2 capture process.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yanan Jiang,Yanbin Yun,Lihua Wang,Min He,Zhi Qiu,ZuYu Li
Polybenzimidazole (PBI) membranes have attracted considerable attention in the energy sector for their outstanding performance. Nevertheless, their development is often restricted by low ionic conductivity. Coordinating metal ions (Fe 3+ ) with PBI can expand the spacing between polymer chains, creating nano-scale ion channels that enhance OH - transport within the membranes. In this study, we fabricated mPBI@Fe coordination membranes using the solution casting method. By varying the iron content, the ionic conductivity of these membranes was regulated. The findings revealed that the conductivity of OH - in these membranes was approximately 61.81 % higher than that of the original mPBI membranes, and they demonstrated excellent mechanical and thermal stability. Furthermore, compared to the commercial FAA-3–50 membrane, the [email protected] membrane demonstrates higher carbon monoxide (CO) fraction current density at a voltage of 3.0 V in the membrane-electrode assembly (MEA). Notably, at 50 mA cm -2 , the Faraday efficiency (FE CO ) of the [email protected] membrane electrodes remained above 95 %. Even after 870 min of electrolysis at 100 mA cm -2 , the FE CO decreased by only 1.57 %. These findings suggest promising prospects for advancing high-performance PBI-based membranes in electrochemical carbon dioxide reduction applications.
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AICHE JOURNAL
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2025
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IF 4
Weilin Li,Rui Ma,Zheyang Liu,Zhehao Liu,Min Zhou,Baker Rhimi,Qiang Ma,Zhifeng Jiang,Weidong Shi
The insufficient light absorption capacity and severe photogenerated carrier recombination limit the overall efficiency of photocatalysts. Herein, we designed carbon-rich poly(heptazine imide) (PHI) by copolymerization of melamine and 2,4,6-triamine-pyrimidine with KCl/KI. This material has been demonstrated to markedly enhance the utilization rate of photons while simultaneously optimizing the charge efficiency of photogenerated electrons. The carbon-rich PHI showed a higher CO₂ reduction efficiency than the PHI, with a CO generation rate reaching 46.6 μmol g −1 h −1 . To overcome the obstacle of slow mass transfer, a flow reactor was designed in-house. The CO yield on carbon-rich PHI in the home-built flow reactor was found to be as high as 153 μmol g −1 h −1 , which is 3.3 times that observed in the batch reactor. The findings of the experimental study are in alignment with the results of the theoretical modeling, which was based on the finite volume analysis method.
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COLLOID AND POLYMER SCIENCE
·
2024
·Vol. 302
·期 7
·1011-1023
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IF 2.2
Yang Haiyan,Gong Yue,Wang Xinzhong,Chen Yuanyuan,Yu Dajiang
Polymer resin-based solid amine are prospective adsorbents used in removing CO 2 from biogas. Two commercial resins with different porous structures, AB-8 and ADS-17, were selected as supports to explore the influence of the support structures on adsorbent performance. It was discovered that macroporous channels greatly boost CO 2 adsorption at higher PEI loadings (≥ 30%), and their influence is more critical than total pore volume or specific surface area, though their impact is minimal at low PEI loadings. ADS-17-40% PEI demonstrated outstanding CO 2 adsorption of 208 mg·g −1 in its 16th cycle under specific operating conditions. Increasing gas flow rate to 200 mL·min −1 could promote CO 2 adsorption capacity and initial adsorption rate constant ( k 0 ) calculated by the deactivation model. The highest adsorption capacity was achieved at 55 °C, when the temperature ranged from 25 to 90 °C. Graphical abstract
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Journal of Environmental Chemical Engineering
·
2024
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IF 7.4
Xuewei Tu,Yutong Chen,Can Sun,Yang Hu,Shouxin Zhu,Jingyi Qu,Zhexiao Zhu,Shijie Zhang,Hui Zheng
The utilization of CO 2 as an economical C1 feedstock for the production of valuable fine chemicals is widely recognized as a green and environmentally friendly approach. In this work, iron/cobalt oxide nanowires (FCO@NWs) composites were synthesized by a simple, convenient and cost-effective hydrothermal process. The FCO@NWs catalyst demonstrated efficient CO 2 fixation with o -phenylenediamine to produce benzimidazole at atmospheric pressure and 150 ℃. After 12 h reaction, the conversion rate of o -phenylenediamine reached an impressive 98%, indicating the catalyst's high efficiency in CO 2 fixation process. Through orthogonal experiments, the optimal reaction condition was confirmed and the application of the FCO@NWs catalyst for various o -phenylenediamine derivatives by substrate expansion was screened. Notably, this catalyst exhibited easy recoverability and reusability without significant loss in catalytic activity even after five cycles of experimentation. This study presents a promising approach for fixing CO 2 into valuable benzimidazole derivatives and contributes some experience to sustainable chemistry.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2024
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IF 11.2
Mengyao Xu,Fei Liu,Shike Liu,Jun Ma,Mengqin Yao,Xiaodan Wang,Jianxin Cao
Metal-based catalysts are prevalent in the CO 2 hydrogenation to methanol owing to their remarkable catalytic activity. Herein, Ru/In 2 O 3 catalysts with different morphologies obtained by doping Ru into In 2 O 3 with irregular, rod-like, and flower-like morphologies are used for catalytic CO 2 hydrogenation to methanol. Results indicate that the flower-like Ru/In 2 O 3 (Ru/In 2 O 3 -F) exhibits higher catalytic performance than Ru/In 2 O 3 with other morphologies, achieving a 12.9% CO 2 conversion, 74.02% methanol selectivity, and 671.36 mg MeOH ·h −1 ·g cat −1 methanol spatiotemporal yield. Furthermore, Ru/In 2 O 3 -F maintains its catalytic stability over 200 h at 5 MPa and 290 °C. The promotional effect mainly stems from the fact that electronic structure of Ru can be effectively adjusted by modulating the morphology of In 2 O 3 . The strong interaction between atomically dispersed Ru and In 2 O 3 -F enhances the structural stability of Ru, inhibiting the agglomeration of the catalyst during the reaction process. Furthermore, density-functional theory calculations reveal that highly dispersed Ru atoms not only perform efficient and rapid electronic gain and loss processes, facilitating the catalytic activation of H 2 into H intermediates. It also enables the generated reactive H to rapidly overflow to the surrounding In sites to participate in CO 2 reduction. These findings provide a theoretical basis for the development of high-performance catalysts for CO 2 hydrogenation.
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Nano Today
·
2024
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IF 13.2
Xiaoxiong Huang,Shengli Wu,Zhichang Xiao,Linjie Zhi,Bin Wang
We report a diatomic-site catalyst configuration constituted by Ni-N 3 and Bi-N 4 embedded in ultrathin nitrogenated carbon nanosheets (Ni/Bi-N-C) which showed dramatically improved activity and selectivity for the conversion of CO 2 to CO. Specifically, the catalyst exhibited high CO Faradaic efficiency (FE CO ) of above 90 % over a wide potential window from −0.76 to −2.22 versus reversible hydrogen electrode with the maximum CO partial current density up to 312 mA cm −2 in a flow cell, and coupled with robust durability. Ni/Bi-N-C-based membrane electrode assembly (MEA) device presented ultrahigh FE CO of 95.7 % at 750 mA and over 100 h of continuous operation without decay under constant current density of 100 mA cm −2 . Mechanistic studies and density functional theory calculations reveal that regulating the CO 2 RR catalytic performance via nearby Ni and Bi active sites can potentially break the activity benchmark of the single metal counterparts because the neighboring Ni and Bi active sites work in synergy to decrease the reaction barrier for the formation of *COOH and desorption of *CO. This work presents an efficient combination of two metal atomic sites which was designed by optimizing the interaction between the atomic sites and key reaction intermediates, resulting in the high-rate electrocatalytic CO 2 reduction.
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