Journal of Energy Chemistry
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2023
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IF 13.1
Zhengrong Liu,Jun Zhou,Yueyue Sun,Xiangling Yue,Jiaming Yang,Lei Fu,Qinyuan Deng,Hongfei Zhao,Chaofan Yin,Kai Wu
Solid oxide electrolysis cell (SOEC) could be a potential technology to afford chemical storage of renewable electricity by converting water and carbon dioxide. In this work, we present the Ni-doped layered perovskite oxides, (La 4 Sr n −4 ) 0.9 Ti 0.9 n Ni 0.1 n O 3 n +2 with n = 5, 8, and 12 (LSTNn) for application as catalysts of CO 2 electrolysis with the exsolution of Ni nanoparticles through a simple in-situ growth method. It is found that the density, size, and distribution of exsolved Ni nanoparticles are determined by the number of n in LSTNn due to the different stack structures of TiO 6 octahedra along the c axis. The Ni doping in LSTNn significantly improved the electrochemical activity by increasing oxygen vacancies, and the Ni metallic nanoparticles afford much more active sites. The results show that LSTNn cathodes can successfully be manipulated the activity by controlling both the n number and Ni exsolution. Among these LSTNn (n = 5, 8, and 12), LSTN8 renders a higher activity for electrolysis of CO 2 with a current density of 1.50A cm −2 @2.0 V at 800 °C It is clear from these results that the number of n in (La 4 Sr n −4 ) 0.9 Ti 0.9 n Ni 0.1 n O 3 n +2 with Ni-doping is a key factor in controlling the electrochemical performance and catalytic activity in SOEC.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Qiang Sun,Hongxia Gao,Teerawat Sema,Zhiwu Liang
High energy consumption during the carbon dioxide (CO 2 ) desorption process in amine-based CO 2 capture technology is a crucial hindrance to achieving carbon neutrality. HZSM-5 is one of the most widely reported solid acid catalysts used in primary amine regeneration. This work compared a series of HZSM-5 zeolites with different Si/Al ratios in terms of CO 2 desorption performance. To further enhance catalytic activity, hierarchical HZSM-5 was synthesized by the dealumination and desilication re-assembly method with different acid and alkali concentrations. The experimental results suggested that desilication by modification in sodium hydroxide resulted in a significant improvement of mesoporous surface area. The NaOH-0.4 catalyst could improve the amount of desorbed CO 2 by 40.3% and decrease the relative heat duty by 28.5%. And the cyclic tests revealed that catalytic activity was well preserved in the recycling process. Moreover, the structure and acidity of modification samples were characterized by X-Ray diffraction (XRD), Fourier transforms infrared (FT-IR), Nitrogen adsorption–desorption experiment, temperature programmed desorption of ammonia (NH 3 -TPD), Pyridine-adsorption infrared spectroscopy (Py-IR), and scanning electron microscopy (SEM). The characterization results suggested that the synergistic effect of larger mesoporous surface area and total acid sites was important to enhance catalytic CO 2 desorption performance. These results showed a new understanding of catalyst design for CO 2 capture technology by modifying the structure of the catalyst support.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2023
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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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Catalysts
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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
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2023
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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
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2023
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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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INORGANIC CHEMISTRY
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2023
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IF 4.6
Shanshan Wu,Meng Tian,Yang Hu,Nan Zhang,Wei Shen,Jianyi Li,Linchuan Guo,Pengfei Da,Pinxian Xi,Chun-Hua Yan
Formate is identified as economically viable chemical fuel from electrochemical carbon dioxide reduction. However, the selectivity of current catalysts toward formate is limited by the competitive reaction such as HER. Herein, we propose a CeO2 modification strategy to improve the selectivity of catalysts for formate through tuning of the *OCHO intermediate, which is important for formate production.
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高影响因子
MOLECULES
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2023
·Vol. 28
·期 5
·2272
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IF 4.6
Zhangxi Gao,Mei Xiang,Mingyang He,Weiyou Zhou,Jiayao Chen,Jiamin Lu,Zeying Wu,Yaqiong Su
Catalytic conversion of CO2with the surplus glycerol (GL) produced from biodiesel manufacturing has attracted much academic and industrial attention, which proves the urgent requirement for developing high-performance catalysts to afford significant environmental benefits. Herein, titanosilicate ETS-10 zeolite-based catalysts with active metal species introduced by impregnation were employed for coupling CO2with GL to efficiently synthesize glycerol carbonate (GC). The catalytic GL conversion at 170 °C miraculously reached 35.0% and a 12.7% yield of GC was obtained on Co/ETS-10 with CH3CN as a dehydrating agent. For comparison, Zn/ETS- Cu/ETS-10, Ni/ETS-10, Zr/ETS-10, Ce/ETS-10, and Fe/ETS-10 were also prepared, which showed inferior coordination between GL conversion and GC selectivity. Comprehensive analysis revealed that the presence of moderate basic sites for CO2adsorption-activation played a crucial role in regulating catalytic activity. Moreover, the appropriate interaction between cobalt species and ETS-10 zeolite was also of great significance for improving the glycerol activation capacity. A plausible mechanism was proposed for the synthesis of GC from GL and CO2in the presence of CH3CN solvent over Co/ETS-10 catalyst. Moreover, the recyclability of Co/ETS-10 was also measured and it proved to be recycled at least eight times with less than 3% decline in GL conversion and GC yield after a simple regeneration process through calcination at 450 °C for 5 h in air.Keywords:CO2;glycerol;glycerol carbonate;ETS-10 zeolite;cobalt-based catalyst
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JOURNAL OF MOLECULAR LIQUIDS
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2023
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IF 6
Wenjian Yue,Xiaojiang Li,Junhao Jing,Jie Qi,Shanshan Dai,Hongsheng Lu,Zhiyu Huang
Hydrocarbon pollutants are not only serious environmental hazards in the exploitation of petroleum resources, but also lead to incomplete utilization of resources. At present, a green solvent called deep eutectic solvents (DES) gradually replaces traditional organic solvents to recover petroleum hydrocarbons, but its recovery still needs to be optimized. For this reason, hydrophobic DES with hydrophilic and hydrophobic properties that can be controlled by CO 2 was developed using fatty acid (FA) as raw material. In the process of using liquid FA to drop into solid FA to prepare DES with an adjustable melting point, DCS technology was used to accurately obtain the melting point and latent heat of the experimental reagent FAs, and the solid − liquid diagram of DES was predicted. Interestingly, the DES prepared by the addition of solid FA and liquid FA retains its strong hydrophobic properties, while the viscosity and melting point can be significantly reduced. FA can transform from oil-soluble physical property to water-soluble physical property by electrostatic binding to polyether amine (D230). This weak non-covalent bond force can be dissociated by CO 2 stimulation, FA can be restored to oil-soluble state, and D230 in aqueous phase can be reduced by removing CO 2 by heating or bubbling N 2 . The reversible pH transformation of the system and 1 H NMR confirm this CO 2 -switchable behavior. In addition, sustainable oil separation (kerosene) was successfully achieved with a maximum oil recovery of 94.6%. Therefore, the novel FA-based DES is expected to be used as an effective extractant for the sustainable clean recovery of hydrocarbons from petroleum resources.
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ENERGY
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2023
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IF 9
Yunzhao Guo,Huiping Zhang,Kaiyun Fu,Xianfu Chen,Minghui Qiu,Yiqun Fan
Amine-based absorption has matured into an established technology for CO 2 capture from fossil fuel power plants. However, high energy consumption for CO 2 desorption remains a challenge. Herein, we report a promising integration of a solid acid catalyst (i.e., HZSM-5) filled into a vapor permeable-liquid impermeable tubular α-Al 2 O 3 ceramic membrane for boosting CO 2 desorption from aqueous monoethanolamine (MEA) solution. Experiments were conducted to investigate the effects of catalyst weight, temperature, pressure, liquid flow rate and CO 2 loading on CO 2 desorption rate and energy consumption. Furthermore, 60 runs of cyclic tests were carried out to assess the stable CO 2 desorption rate and the thermal and chemical stability of both the HZSM-5 catalyst and the α-Al 2 O 3 membrane. The experiment results demonstrated that the HZSM-5 filled α-Al 2 O 3 ceramic membrane contactor exhibited high CO 2 desorption performance and long-term stability. It is anticipated that integration of solid acid catalyst with porous ceramic membrane holds great promise in practical application to boost the CO 2 desorption rate and reduce the energy requirement.
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JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Sihui Li,Keming Zhang,Chenlu Liu,Xiaoting Feng,Peijin Wang,Shaofei Wang
Polymeric membranes containing polyethylene oxide (PEO) groups are promising CO 2 separation materials, but suffer from the trade-off between separation performance and mechanical strength . To overcome this challenge, we combine the merits of semi-interpenetrating polymer network and nanohybrid to maintain a high PEO loading and robust membrane structure. The membranes were prepared by introducing in-situ formed PEO networks with silica nodes into Pebax1657 to produce a semi-interpenetrating network structure. The introduced network and in situ formed silica nanoparticles reduce the chain packing efficiency of Pebax matrix to enhance the CO 2 diffusivity , while the increased PEO content enhances CO 2 solubility. Under feed gas pressure of 25 bar, nanohybrid membranes containing 40 wt% polymer network display excellent gas separation performance with CO 2 permeability of 272.8 Barrer and CO 2 /N 2 selectivity of 79.6 under mixed gas separation tests, surpassing 2008 Robeson upper bound. Moreover, the hybrid membranes showed high mechanical strength, the Young's modulus increases by 1.95 times. This strategy provides a simple route for the design of nanohybrid membranes with high separation performance as well as excellent durability.
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
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2023
·Vol. 27
·期 5
·1261-1268
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IF 2.5
Deng Hao-chen (Preston),Hao Qingzhu,Wang Yuhang
The COVID-19 pandemic that is still prevalent around the globe each day consumes massive disposable face masks and consequently lays a heavy burden on waste management. Meanwhile, the incineration of these medical wastes further escalates the already overwhelming carbon emission that leads to global warming and climate change. To offer a potential solution addressing medical waste and CO 2 emission challenges, we herein develop a synthetic protocol to upgrade face masks into Ni, N-doped graphene (Ni–N-C) sheet catalysts for selectively reducing CO 2 into CO electrochemically. The high specific surface area and the uniform dispersion of Ni active sites of the catalyst derived from a regular disposable face mask enable a near-unity CO Faradaic efficiency (FE) at the current density of 200 mA cm −2 . This study offers outside-of-the-box thinking to address environmental issues by turning medical wastes into CO 2 reduction catalysts.
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