CHEMISTRY OF MATERIALS
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2022
·
IF 10.508
Qian Liang,Yu Zhao,Jian-de Chen,Jia-jun Dai,Xingyu Ding,Zhen Tong,Shi-jun Xie,Jing Zhang,Zhe-hui Zhou,Jun-Tao Li,Jian-Feng Li,Yao Zhou
Anti-perovskites represent a type of newly arising functional materials with a well-defined cubic lattice crystal structure; they provide an excellent entity for studying structure–activity relationship in heterogeneous catalysis. Herein, nitride-based anti-perovskite CuNNi3 was synthesized, and its catalytic properties in electroreduction of carbon dioxide (CO2RR) to syngas were explored for the first time. The introduction of N into the body center of the face-centered cubic cell of CuNi3 was found to create abundant Lewis basic sites with various strengths and thus favored stronger adsorption of the relevant critical species, thus leading to significant improvement in the efficiency of CO2RR and hydrogen reduction compared with that of CuNi3. More importantly, when a thin CuNNi3 nanoshell is coated on a CuNi3 alloy core, significant nanosizing and interfacial interaction effects are noticed, which change the catalytic behaviors of the anti-perovskite. On one hand, the nanosizing effect leads to occurrence of Ni2+ species with a higher oxidative state and consequently deactivates the weak Lewis basic sites in the CuNNi3 nanoshell, which accordingly inhibits hydrogen evolution; the CuNi3@CuNNi3 nanocomposite thus delivers CO Faradaic efficiency up to 96% in comparison to a value of 70% yielded by the bulky counterpart. On the other hand, evident interfacial electron delocalization from the CuNi3 alloy core to the CuNNi3 nanoshell was observed, which was found to increase the N escape energy in the cubic cell of CuNNi3 and consequently enhance its chemical stability; as a result, the CuNi3@CuNNi3 nanocomposite displays much improved catalytic stability compared with the bulky counterpart in CO2RR. This work for the first time explores the interesting electrocatalytic behavior of nitride-based anti-perovskites in electrochemical reduction of CO2, which spells a grand opportunity for the structure–relationship study in CO2RR.
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DOI
高影响因子
CERAMICS INTERNATIONAL
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2018
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IF 3.057
Yingchao Hu,Wenqiang Liu,Yuandong Yang,Xianliang Tong,Qianjun Chen,Zijian Zhou
Li 4 SiO 4 sorbents for high-temperature CO 2 removal have drawn extensive attention owing to their potential application in carbon capture and storage (CCS). The major challenge in the application lies in the poor CO 2 capture performance under realistic conditions of low CO 2 concentrations, owing to the dense structure and poor porosity. In this work, Li 4 SiO 4 sorbents were prepared with porous micromorphologies and large contact areas using a variety of organometallic Li-precursors, achieving fast CO 2 sorption kinetics, high capacity and excellent cyclic stability at a low CO 2 concentration (15 vol%). It was found that a high conversion of ~ 74% was maintained for pure Li 4 SiO 4 even after 100 sorption/desorption cycles. Moreover, by doping with Na 2 CO 3 to reduce the CO 2 diffusion resistance, the conversion of the sorbent was further enhanced to 93.2%. The enhancement mechanism of alkali carbonate have been proven here to be ascribed to the formation of the eutectic melt of Li/Na carbonates, the existence and function of which has been confirmed in this study.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Lingfei Liu,Mingshan Zhang,Zhouguang Lu,Zhehui Jin,Yi Lu,Dejun Sun,Zhenghe Xu
Hypothesis Pseudo-Gemini surfactants (PGS) possessing switchable and recyclable features have drawn increasing attention on generating high-performance CO 2 -responsive emulsions for wide range and versatile applications. However, there is a lack of fundamental understanding on how the molecular structure of PGS affects the stability and switchability of emulsions. We hypothesize that the length and type of the spacer in PGS play a decisive role in controlling interfacial and switching properties. Experiments Two series of PGS with different spacers were prepared through electrostatic association between amines and oleic acid . The interfacial activity and CO 2 -responsive properties of corresponding emulsions were systematically investigated by well-designed experiments and molecular dynamics simulations . Findings Increasing the spacer length to allow the bent configuration leads to more tight arrangement of oleic molecules, consequently improving the interfacial activity. In addition, the introduction of amino group into the spacer dramatically promotes CO 2 response of resulting PGS due to ehanced migration of the spacer from the interface to the aqueous phase after CO 2 addition. These results are inspiring in designing controllable CO 2 -responsive emulsions for a wide range of industrial applications ( e.g. , enhanced oil recovery and oil-contaminated soil remediation).
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
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IF 11.357
Yichao Tong,Changlei Qin,Linyan Zhu,Shuzhen Chen,Zongze Lv,Jingyu Ran
The huge consumption of fossil fuels leads to excessive CO2 emissions, and its reduction has become an urgent worldwide concern. The combination of renewable energies with battery energy storage, and carbon capture, utilization, and storage are well acknowledged as two major paths in achieving carbon neutrality. However, the former route faces the discard problem of a large amount of lithium-ion batteries (LIBs) due to their limited lifespan, while it is costly to obtain effective CO2-capturing materials to put the latter into implementation. Herein, for the first time, we propose a route to synthesize low-cost Li4SiO4 as CO2 sorbents from spent LIBs, verify the technical feasibility, and evaluate the CO2 adsorption/desorption performance. The results show that Li4SiO4 synthesized from the cathode with self-reduction by the anode graphite of LIBs has a superior CO2 capacity and cyclic stability, which is constant at around 0.19 g/g under 15 vol % CO2 after 80 cycles. Moreover, the cost of fabricating sorbents from LIBs is only 1/20–1/3 of the conventional methods. We think this work can not only promote the recycling of spent LIBs but also greatly reduce the cost of preparing Li4SiO4 sorbents, and thus could be of great significance for the development of CO2 adsorption.
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高影响因子
APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Changchun Ji,Yudong Wang,Ning Zhao
Cu Al hydrotalcite-SBA-15 composite materials are prepared by precipitation-deposition method. The CO 2 adsorption and regeneration process are carried out in a fixed bed reactor . This composite has thermal stability derived from hydrotalcite and moderate regeneration temperature from the porous material SBA-15. The adsorption capacities of the composite are obviously improved compared to the pure SBA-15 or hydrotalcite. When the amount of hydrotalcite is increased to 40 wt%, it has the magnitude of adsorption capacity. The inactivation model can well simulate the CO 2 adsorption process of the composite.
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DOI
高影响因子
Chemistry-An Asian Journal
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2019
·Vol. 15
·期 15
·2364-2370
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IF 3.698
Guozhen Liu,Long Cheng,Guining Chen,Feng Liang,Gongping Liu,Wanqin Jin
Mixed matrix membranes (MMMs) made from inorganic fillers and polymers is a kind of promising candidate for gas separation. In this work, two-dimensional MXene nanosheets were synthesized and incorporated into a polyether-polyamide block copolymer (Pebax) matrix to fabricate MMM for CO 2 capture. The physicochemical properties of MXene nanosheets and MXene/Pebax membranes were studied systematically. The introduction of MXene nanosheets provided additional molecular transport channels and meanwhile enhanced the CO 2 adsorption capacity, thereby enhancing both the CO 2 peremance and CO 2 /N 2 selectivity of Pebax membrane. The optimized MXene/Pebax membrane with a MXene loading of 0.15 wt % displayed a high separation performance with a CO 2 permeance of 21.6 GPU and a CO 2 /N 2 selectivity of 72.5, showing potential application in CO 2 capture.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Dun Zhou,Hongbo Zhang,Yulong Rao,Xiaobai Li,Huihui Zhang,Yongpeng Liu,Hongwei Ma
CO 2 capture and release are critical for enhancing photosynthetic efficiency of plants and biomass accumulation. However, achieving efficient capture and directional transport of CO 2 to plants near the source of carbon emissions to boost photosynthetic efficiency are mains an important technical challenge. In this study, we introduce an innovative strategy for fabricating a cellulose-based CO 2 -capture foam-like porous material-DGP, which can significantly enhance the photosynthetic efficiency of tobacco plants. By chemically crosslinking superbranched amino polymers on a lignocellulose substrate, DGP not only exhibits excellent CO 2 capture capacity of 8.01 mmol g −1 at room temperature, but also achieves an effective slow release of CO 2 with a release rate of up to 51 % and a duration of up to 10 h without additional energy input. This characteristic allows DGP to simulate the CO 2 concentration mechanism of plants in nature, thereby increasing the net photosynthetic efficiency of tobacco by 70 % and the intercellular CO 2 concentration by 52 %, which significantly promotes the accumulation of biomass. The utilization of this material has broad application prospects for enhancing the carbon sink capacity of the ecosystem, mitigating the greenhouse effect and improving crop yield.
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Qiang Li,Yuhang Ding,Teng Wang,Zhuo Xiong,Junying Zhang,Yongchun Zhao
Dual-function amine-based electrolytes provide both carbon dioxide (CO 2 ) capture and electrocatalytic CO 2 reduction capabilities, combining the capture and conversion steps of conventional separations in a single system, increasing efficiency and reducing energy consumption. Cations serve as critical constituents within bifunctional amine-based electrolytes, integral to both CO 2 absorption mechanisms and the electrochemical reduction of carbamates, but this issue has not been comprehensive studied. In this study, we investigated the effect of five different cations (M + = Li + 、Na + 、K + 、Rb + 、Cs + ) on the CO 2 capture and electroreduction properties of dual-function amine-based electrolyte. Electrochemical comparative analyses reveal that the presence of larger cations (Cs + ) significantly reduces series resistance and charge-transfer resistance, while augmenting electric double-layer capacitance and electrochemical surface area. These synergistic effects culminate in elevated current densities and accelerated reaction rates during carbamate reduction processes. Density functional theory (DFT) simulations elucidate that expanding cationic radii strengthen both adsorption trends and charge transfer of carbamate (R 1 R 2 NCOO - ) at electrode–electrolyte interface. Comparative analysis of the HOMO-LUMO orbitals shows that R 1 R 2 NCOO - Cs + is more easily reduced and electronic excited. These computational validate the observed enhancements in current density from experimental electrochemical. Higher electrolyte concentrations (≥1 M) enhance the selectivity of carbamate reduction but impede mass transfer due to increased viscosity following CO 2 absorption. Conversely, lower electrolyte concentrations (<1 M) improve the current density of carbamate reduction but reducing CO 2 capture rates. Moreover, an equimolar cation-to-amine optimizes the enhancement of CO 2 absorption capacity and electroreduction efficiency. This work provides a comprehensive understanding of how cations influence the electrocatalytic reduction of captured CO 2 in amine-rich solutions, offering valuable insights for the design of electrolytes for CO 2 capture and electroreduction.
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高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Shang-Yuan Cheng,Chen-Peng Zhang,Meng-na Chao,Shu-Wei Guo,Gui-Sheng Qi
Suspended nanodroplets affect the transfer process within fluids through micro-perturbation or micro-convection effects. Therefore, adding dispersed nanodroplets as the dispersed phase into the liquid phase to form nanoemulsions can enhance the CO 2 absorption process. The quality of nanoemulsions mainly depends on the emulsification equipment. Traditional physical mechanical effects can only achieve large-scale macroscopic mixing, which usually takes a long time to complete, resulting in issues such as low production efficiency, batch operation, and long preparation cycles. This paper uses an impinging stream-rotating packed bed as a reactor, with span60 and tween60 as surfactants, and adopts a high-gravity process intensification technology to prepare undecane/methanol nanoemulsions with good dispersion stability. Nanoemulsion absorbents for CO 2 capture applications have been developed. The effects of different operating conditions on the dispersion stability of nanoemulsion were investigated. Furthermore, CO 2 absorption performance of nanoemulsion absorbents and methanol were investigated in a bubbling reactor. Based on the results, the reasonable mechanism for the enhancement of mass transfer was also discussed in detail. Further experiments on CO 2 absorption using nanofluids were conducted and compared with pure methanol. The results indicate that when the undecane volume fraction is 0.01 %, the high-gravity factor is 27, the impinging velocity is 14.1 m·s −1 , and the circulation time is 20 min, the nanoemulsion exhibits the highest stability, with the narrowest particle size distribution of oil droplets, an average particle size of 20.5 nm, and the highest uniformity. Simultaneously, the change in turbidity over time is minimal. The corresponding thermal conductivity at 25°C is 0.2003 W/m·K. The addition of nano-oil droplets significantly accelerates the CO 2 absorption rate, allowing the absorbent to reach saturation earlier, while the total amount of CO 2 absorbed remains the same. Compared with pure methanol, the nanoemulsion enhances the CO 2 absorption rate by 4.48 %. This work may provide a promising green method for efficient production of nanoemulsions for carbon dioxide capture.
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Xiaoqiang Wang,Menghan Li,Zhiyuan Liu,Zhuang Shi,Daoyong Yu,Baosheng Ge,Fang Huang
Utilizing carbonic anhydrase (CA) to catalyze CO 2 hydration offers a sustainable and potent approach for carbon capture and utilization. To enhance CA's reusability and stability for successful industrial applications, enzyme immobilization is essential. In this study, delignified bamboo cellulose served as a renewable porous scaffold for immobilizing CA through oxidation-induced cellulose aldehydation followed by Schiff base linkage. The catalytic performance of the resulting immobilized CA was evaluated using both p -NPA hydrolysis and CO 2 hydration models. Compared to free CA, immobilization onto the bamboo scaffold increased CA's optimal temperature and pH to approximately 45 °C and 9.0, respectively. Post-immobilization, CA activity demonstrated effective retention (>60 %), with larger scaffold sizes (i.e., 8 mm diameter and 5 mm height) positively impacting this aspect, even surpassing the activity of free CA. Furthermore, immobilized CA exhibited sustained reusability and high stability under thermal treatment and pH fluctuation, retaining >80 % activity even after 5 catalytic cycles. When introduced to microalgae culture, the immobilized CA improved biomass production by ∼16 %, accompanied by enhanced synthesis of essential biomolecules in microalgae. Collectively, the facile and green construction of immobilized CA onto bamboo cellulose block demonstrates great potential for the development of various CA-catalyzed CO 2 conversion and utilization technologies.
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Lihang Yan,Guanhua Liu,Jianqiao Liu,Jing Bai,Yaoxuan Li,Huaxun Chen,Liya Zhou,Jing Gao,Yanjun Jiang
The utilization of CO 2 has become an important issue aiming to the achievement of carbon neutrality. The enzyme electrocatalytic CO 2 reduction to produce carbonaceous fuels has been increasingly appealing. While the low CO 2 aqueous solubility severely limits the CO 2 reduction efficiency, and the expensive cofactor restricts the application potential. In this study, microporous UiO-66-NH 2 was firstly converted into hierarchically porous structure (HP-UiO-66-NH 2 ) containing both micropores and mesopores to simultaneously enhance the enrichment of CO 2 and the immobilization of formate dehydrogenase by optimizing the pore structure. The relative contents of the protein secondary structures were similar after immobilization. The mechanism of enzyme electrocatalytic CO 2 reduction was proposed. The enzyme stability was highly enhanced after immobilization and the CO 2 reduction was enhanced by the enzyme electrocatalytic system through the combination of CO 2 enrichment and electrocatalytic NADH regeneration. The optimized catalytic system can obtain formate yield of 1.826 mM in 3 h (5.57 times higher than the free enzyme system) with a generation rate of 6086.7 μmol g cat ‑1 h ‑1 .
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Zheng Lian,Youcai Lu,Shiyu Ma,Liqin Wang,Zhongjun Li,Qingchao Liu
In Li-CO 2 battery, redox mediators (RMs) are considered to have bright prospects due to their advantages of optimizing the mediated reaction pathway and reducing over-potential. However, some inherent defects caused by RMs, such as induced Li anode degradation and electron shuttle, limit its application in Li-CO 2 battery. In this work, ruthenium acetylacetonate (Ru(acac) 3 ) was innovatively applied as an efficient RM to boost the performance of Li-CO 2 battery, and the “shuttle effect” of Ru(acac) 3 to Li anode was also confirmed. To avoid the anode degradation caused by “shuttle effect” of RM, a novel Zn-MOF nanoplate modified glass fiber (M-GF) separator is skillfully prepared and used as a dual-function separator for Li-CO 2 battery. Experiments coupled with density functional theory simulations verifies that M-GF can protect Li anode by preventing Ru(acac) 3 from entering Li anode by physical and chemical interactions. Moreover, the highly ordered micropores in Zn-MOF also induce uniform deposition of Li + on the Li anode to delay the degradation process of anode, and thus prolonged the cycle life of the battery. Thanks to the bidirectional support of Ru(acac) 3 and M-GF strategy, the electrochemical performances of the Li-CO 2 battery, especially the round-trip efficiency and cycle life, has been greatly improved.
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高影响因子
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