SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Huihui Ding,Huanhuan Wu,Jun Ma,Xiang Li,Shuangshuang Huai,Chengming Zhang,Haibao Zhu,Ping Li,Jie Li,Xiufang Wang,Wenjie Xie
Artificial photosynthesis converting CO 2 into valuable compounds has garnered significant interest. However, the insufficient surface activity sites, weak adsorption capacity of CO 2 and poor electron-hole separation capability hinder CO 2 photoreduction used for practical implementation. Herein, Bi nanoparticles/Bi 24 O 31 Br 10 composite photocatalyst (Bi/BOB) was designed constructed through in-situ reduction of bismuth metal on the surface of ultra-thin Bi 24 O 31 Br 10 nanosheets. Bi/BOB exhibits an excellent ability to reduce CO 2 to CO. The CO 2 reduction rate of the optimized Bi/BOB composite catalyst is 43.07 μmol·g −1 ·h −1 , which is significantly superior to other reported bismuth-based photocatalysts. Experimental characterization and Theoretical simulation calculation reveal that the in-situ reduction of bismuth metal causes significant local lattice distortion and uneven charge distribution, thereby producing a strong interaction between Bi nanoparticles and BOB support. So, it enhances the adsorption and activation of carbon dioxide molecules and reduces the Gibbs free energy barrier during the catalytic reaction. Moreover, the strong interaction helps to enhance the separation of photogenerated charge carriers and stability of catalysts. This study offers research suggestions for the interaction between metal and support to enhance CO 2 reduction.
✓ 已验证
产品关联
DOI
高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 22
·e202401690
·
IF 1.9
Menghan Xue,Fazhan Li,Zhen Li,Yuxia Sun,Yiping Guo,Yuehui Li
Graphical Increase of graphitic-N doping and graphitization degree of outside shells encapsulating Ni nanoparticles was developed to efficiently promote cathodic reduction of CO 2 to CO. Despite of high conductivity and reducing ability, transition metal nanoparticles tend to aggregate and unavoidably impact the selectivity during the proton-coupled reduction process of CO 2 RR. New strategy to regulate and utilize the electronic property of transition-metal particles allows for effective tuning of eCO 2 RR activity. Through simple creation of N-doped carbon shells surrounding Ni nanoparticles and controlling the amount and arrangement of the N atoms, successful and long-lasting electrochemical reduction of CO 2 was accomplished. The inherent HER activity was almost completely suppressed. It exhibited FE CO above 90 % in a 500 mV potential window, with the optimal up to 96.5 % at −0.78 V vs RHE. In flow cell electrolysis, a current density of 289.4 mA/cm 2 was achieved with Faradic efficiency of 96.4 % towards CO. The results of control experiments using different catalysts imply that electron transfer between Ni core and shells was significantly influenced by the property of N atoms. High content of graphitic nitrogen is crucial for the catalytic performance.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Shuzhuang Sun,Bocheng Yu,Yanmei Shen,Yu Liu,Hongman Sun,Xuan Bie,Mengna Wu,Yongqing Xu,Chunfei Wu,Hui Zhou
Integrated CO 2 capture and utilization (ICCU) using “capture-conversion” dual functional materials (DFMs) paves a cost-effective path for restricting CO 2 emissions by eliminating the energy-intensive intermediate processes. The interactions between catalysts and absorbents are believed pivotal in ICCU; however, there is a lack of environment-friendly strategy to fabricate the interaction for industrial applications. Here, we propose a solvent-free mechanochemical approach to promote the interaction by improving the proximity between natural calcium and iron sources. The interaction was systemically investigated and confirmed using XRD, XPS, TEM, TPR, etc. As a result, the mechanochemical approach derived DFM achieved 5.5 mmol g −1 CO 2 capacity, 87 % CO 2 conversion, and 100 % CO selectivity at 650 °C, significantly outperforming the CaO-alone benchmark (CO 2 capacity < 4.5 mmol g −1 , CO 2 conversion < 73 %). Further incorporating MgO would alleviate the sintering and promote the CO 2 capture stability (< 15 % decrease after 20 cycles) by acting as a thermal-stable barrier. Based on in situ XRD, it is further confirmed that Fe-Ca interaction exhibits a dynamic looping mechanism in ICCU. The techno-economic analysis strongly supports the superiority of ICCU catalyzed by naturally sourced DFMs on eliminating the energy and H 2 consumption for CO 2 capture and upgradation. As a result, producing CO via ICCU using mechanochemical derived DFMs exhibits 20 % and 10 % cost decrease compared to the conventional CCU and ICCU using CaO alone scenarios, pointing out the potential of ICCU technology in industrial applications.
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Ziwen Mei,Kejun Chen,Yao Tan,Qiuwen Liu,Qin Chen,Qiyou Wang,Xiqing Wang,Chao Cai,Kang Liu,Junwei Fu,Min Liu
ABSTRACT Electrocatalytic CO 2 reduction reaction (CO 2 RR) holds significant promise for sustainable energy conversion, with cobalt phthalocyanine (CoPc) emerging as a notable catalyst due to its high CO selectivity . However, CoPc's efficacy is hindered by its limited ability to provide sufficient proton for the protonation process, particularly at industrial current densities . Herein, we introduce defect-engineered carbon nanotubes (d-CNT) to augment proton feeding for CO 2 RR over CoPc, achieved by expediting water dissociation. Our kinetic measurements and in-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy reveal d-CNT significantly enhances proton feeding, thereby facilitating CO 2 activation to *COOH in CoPc. Density functional theory calculations corroborate these findings, illustrating that d-CNT decreases the barrier to water dissociation. Consequently, the CoPc/d-CNT mixture demonstrates robust performance, achieving 500 mA cm –2 for CO 2 RR with CO selectivity exceeding 96%. Notably, CoPc/d-CNT remains stability for a duration of 20 h under a substantial current density of 150 mA cm –2 . The study broadens the scope of practical applications for molecular catalysts in CO 2 RR, marking a significant step towards sustainable energy conversion.
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Yingyang Song,Junyu Lang,Qingrui Zeng,Jinping Cheng,Mingce Long
Monoethanolamine (MEA)-based carbon dioxide absorption is one of the effective carbon capture, utilization, and storage (CCUS) technologies but is significantly restricted by the high energy consumption in the regeneration of rich amine solution. Solid acid catalysts have the potential to reduce energy consumption, while the exploration of highly active catalysts with abundant Bro̷nsted and Lewis acid sites remains needing. We developed an efficient solid acid catalyst, niobium-modified HZSM-5 (Nb/HZ), to facilitate CO2 desorption from the CO2-captured MEA solutions. The Nb/HZ catalysts with various niobium loadings were synthesized by using an impregnation method. HZSM-5 retained its pore structure and large surface area after niobium incorporation. The catalyst with 4% Nb (4.0-Nb/HZ) has the highest activity and stability, with 61% increase in the desorption rate, 50% increase in the desorbed CO2 amount, and 37% reduction of relative heat duty. According to theoretic calculations and experimental analyses, the Nb/HZ catalyst provides abundant Bro̷nsted and Lewis acid sites to facilitate carbamate adsorption, proton transfer, and carbamate breakdown, thus reducing the activation energy for CO2 desorption. This work provides a valuable solid acid catalyst for amine-based CO2 capture and also brings insights for the development of a novel solid acid for diverse catalysis.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhipeng Chen,Tao Wang,Chao Li,Mengxiang Fang,Wei Chen,Ximing Hu,Yan Shao,Zhihao Liu,Wei Zhang,Li Zhang,Wenyang Fan,Shaojuan Zeng
Lower regeneration energy and superior cyclic capacity have enabled biphasic absorbents great potential in the area of flue gas CO 2 capture. The liquid film mass transfer coefficient(k L ) is a vital parameter in the development of absorbents with efficient CO 2 absorption mass transfer performance, while the phase separation behavior of biphasic solutions could be an essential factor for the absorption mass transfer and the stability of absorber. However, systemic kinetic research towards biphasic absorbents, especially the impact of phase separation behavior, is limited. In this study, a typical amide-based biphasic absorbent diethylenetriamine(DETA)/diethanolamine(DEA)/N, N-dimethylacetamide(DMAC) which has achieved great reduction in regeneration energy, was selected as the subject of kinetic investigation in a wetted wall column. The CO 2 overall mass transfer coefficient(K G ) of DETA/DEA/DMAC exceeded other biphasic solvents, blended amine solution, and 40% K 2 CO 3 solution, with 3 times that of 40% K 2 CO 3 solution. Moreover, various operational conditions including absorption temperature, gas flow rate, and water content of solution were taken into account to build a multiple-condition kinetic mechanism to offer guidance for biphasic absorbents. Furthermore, phase separation behavior was revealed as the main blame for the deterioration in the liquid film chemical mass transfer process of biphasic solvents in the CO 2 absorption process, resulting in the k L of DETA/DEA/DMAC before phase separation decreased by 75.3% at the phase separation stage. Therefore, it is crucial to ensure that the CO 2 loading of the solution entering absorber is lower than the phase separation point in applications. After phase separation, DETA/DEA/DMAC split into the organic and aqueous phases, the k L of the aqueous phase gradually exceeded that of the organic phase as CO 2 loading increased for its higher chemical enhancement factor(E).
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xiaohong Chen,Wei Zou,Shengke Liang,Hong Wang,Chen Zhang
Adsorbent materials with high adsorption efficiency, good processing stability, and high adsorption rate, are crucial for carbon capture, utilization and storage (CCUS) technology. In this paper, a novel polyethyleneimine (PEI)-embedded porous adsorbent with high amine-content matrix was one-step prepared successfully by a unique high internal phase emulsion (HIPE) polymerization. Firstly, the amphiphilic polyethyleneimine-based carbon nanotubes (CNT-PEI) was synthesized and applied as a Pickering emulsifier, and the interfacial tension was analyzed by a multi-functional tensiometer. Secondly, a large amount of divinylbenzene (DVB) was introduced into the continuous phase of HIPE, and then some mesopores were generated in the framework of the macro-porous polymer, which indicated by specific surface and pore size analyzer and scanning electron microscope (SEM), respectively. Finally, the additional PEI was added into the dispersed phase of HIPE. In such unique HIPE template, PEI was penetrated into the framework and then the porous polymer with high amine-content matrix was achieved. The morphology, the surface element content and the CO 2 adsorption capacity of the obtained porous polymer were characterized by SEM, energy dispersive spectrometry (EDS), and the gas sorption analyzer. When the obtained porous polymer was applied as CO 2 adsorbent, the better comprehensive adsorption performance, including high CO 2 adsorption capacity of 2.87 mmol/g, fast adsorption kinetics, the isosteric heat of adsorption (Q st ) range of 65–68 kJ/mol, exceptional CO 2 /N 2 selectivity with a separation factor up to 118, and stable adsorption–desorption cycles, was exhibited. The superior CO 2 adsorption capacity and adsorption kinetics make it a promising candidate in practical CO 2 adsorption application.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·
IF 2.7
Jiaqi Huang,Jian Zhang,Xiujun Wang,Bo Huang,Zhao Hua,Shenwen Fang
Improving the stability of CO 2 foam is a core concern in CO 2 foam flooding oil recovery technology. Using hydrophobic nano-SiO 2 to enhance the stability of CO 2 foam is a common approach, but hydrophobic nano-SiO 2 faces challenges, such as easy aggregation, difficult dispersion, and performance needs to improve. In this article, a novel dispersion of styrene-phenylamine monomer copolymer (PSSN) nanosphere with primary amine groups on the surface was synthesized. The synthesis conditions of PSSN were optimized, and its performance for stabilizing CO 2 foam was evaluated. The experimental results demonstrated that PSSN had better performance for stabilizing CO 2 foam than that of hydrophobic nano-SiO 2 when using cocamidopropyl betaine (CAB) as the foaming agent. With the CAB concentration of 4000 mg/L and PSSN concentration of 100 mg/L in the brine having salinity of 8460 mg/L, the half-life of CO 2 foam at 90°C was 131 min, which was 43 min longer than that stabilized by hydrophobic nano-SiO 2 under the same conditions. This is for the first time that polystyrene microspheres with amine groups on the surface was used to stabilize CO 2 foam. The study provides a new nanoparticle option for stabilizing CO 2 foam.
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 9
·892
·
IF 4
Zhen Li,Kwang Leong Choy
Electrocatalytic CO2reduction driven by renewable electricity offers a sustainable approach to producing valuable chemicals, though it is often hindered by low activity and selectivity. CuO, an important transition metal oxide, exhibits unique advantages in photoelectrocatalysis due to its high intrinsic catalytic activity and ability to serve as an active site for CO2reduction. SiO2, a widely used substrate, facilitates Cu loading and increases the specific surface area of the catalyst. Meanwhile, g-C3N4provides excellent visible-light responsiveness and efficient charge carrier mobility. Together, CuO, SiO2, and g-C3N4are earth-abundant, low-cost, and chemically stable, making them ideal for solar-to-fuel applications. Here, a novel ternary heterojunction photocatalyst was constructed using SiO2, CuO, and g-C3N4. The heterostructure significantly improves light-harvesting efficiency, promotes efficient charge separation and transport, and simultaneously mitigates photogenerated carrier recombination and catalyst corrosion. The resulting SiO2@CuO/g-C3N4catalyst demonstrates outstanding CO2conversion performance, achieving a CO yield of 17 mmolg−1h−1at 1.2 VRHEwith nearly 100% selectivity. Moreover, this work systematically investigates the electrocatalytic CO2reduction reaction (CO2RR) mechanism on Cu-based catalysts, offering insights into the formation of high-value multicarbon products and highlighting the potential of rational heterojunction design in enhancing solar-driven fuel production efficiency.
✓ 已验证
产品关联
DOI
高影响因子
Joule
·
2024
·
IF 38.6
Jun Wang,Jiajia Wang,Jianyong Feng,Yingfei Hu,Huiting Huang,Ningsi Zhang,Minyue Zhao,Wangxi Liu,Changhao Liu,Zhi Zhu,Shicheng Yan,Tao Yu,Ce Zhang,Wei Yao,Zhigang Zou,Zhaosheng Li
The primary source of oxygen in space exploration is derived from water electrolysis. Herein, we discovered a mild photochemical hydrogenation process that can convert CO 2 into carbon nanotubes (CNTs) and H 2 O by using a Co-based catalyst. Hence, astronauts can extract oxygen from CO 2 metabolism to close the oxygen recycling loop (overall reaction: CO 2 → C + O 2 ), allowing for ∼100% theoretical oxygen recovery. This photochemical technique has enabled a high turnover number (the molar ratio of C to Co) of 240 for CNT formation during a 100 h reaction in a flow reactor. The oxygen recovery efficiency reaches approximately 68% when using flowing CO 2 and H 2 , surpassing the theoretical maximum (50%) for the Sabatier reaction combined with water electrolysis at the International Space Station. The tip-growth mode of CNTs principally allows long-term oxygen recovery from CO 2 , in addition to space manufacturing of CNTs.
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Zongze Lv,Jiaqi Ruan,Weifeng Tu,Xun Hu,Donglin He,Xin Huang,Changlei Qin
Integrated carbon capture and utilization by methanation (ICCU-methanation) is an emerging concept in reducing CO 2 emissions and storing H 2 simultaneously. One key of the technology is the development of dual functional materials (DFMs) that can efficiently capture CO 2 and then catalyze it. Herein, we propose the construction of DFM using Li 4 SiO 4 with superior CO 2 adsorption/desorption features as sorbent and catalyst carrier, CeO 2 as catalyst promoter and isolator, and Ni as catalytic metal, and comprehensively evaluate its characteristics and performance in ICCU-methanation. Results show that the DFM developed possess a high and stable CO 2 capacity of 5.4 mmol·g DFM -1 , 96 % CO 2 conversion and 96 % CH 4 selectivity under both the ideal CO 2 capturing atmosphere and the realistic flue gas containing 10 vol% steam and 8 vol% O 2 . Moreover, rapid CO 2 dissociation from the DFM is observed at a temperature lower to 560 °C due to the reaction of H* dissociated by catalyst with carbonate to form formate, which further decomposes to release CO.
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2018
·
IF 3.024
Dongfang Liu,Yuxin Suo,Jihe Zhao,Peiyao Zhu,Jiang Tan,Baogang Wang,Hongsheng Lu
Acidic substances (naphthenic acids) were found in crude oil, which provides favorable conditions for the formation of surfactants. N,N-Dimethylcyclohexylamine (DMCHA) can activate the naphthenic acid in the crude oil to form the surfactant by noncovalent bonding. This process has an unusual meaning for the crude oil pipelines transportation by the method of forming a low-viscosity oil-in-water emulsion. At the same time, CO2 can be used as a demulsifier to separate crude oil and water at the end of pipeline transportation because the surfactant has a CO2 stimulus response characteristic. In our study, it was found that crude oil-in-water emulsion can be formed and has very good stability. CO2 has a high demulsification efficiency in emulsions with lower crude oil content. For high oil content conditions, the emulsion cannot be demulsified completely by CO2. Since sulfuric acid, hydrochloric acid, and the like are liquid and corrosive, this is not conducive to its application as a demulsifier in crude oil pipeline transportation. Organic acids in this area have a stronger advantage obviously, so citric acid, oxalic acid, acetic acid, and lactic acid were used as demulsifiers in this article; all of them have good demulsification performance in high crude oil content emulsions, especially citric acid. Meanwhile, DMCHA can be recycled and reused by adding NaOH to the lower aqueous solution after demulsification.
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）