Greenhouse Gases-Science and Technology
·
2022
·Vol. 12
·期 3
·362-375
·
IF 2.518
Jinxiu Li,Yu Li,Chen Li,Rui Tu,Pengfei Xie,Yi He,Yao Shi
While nonaqueous organic-amine absorbents have great potential in reducing energy consumption of CO 2 capture, their absorption/desorption behaviors are still poorly understood when high-concentration polyamines are used. On the other hand, large scale CO 2 capture demands the use of high-concentration polyamines absorbents. Therefore, we investigated the absorption and microwave regeneration behavior of high-concentration triethylenetetramine (TETA) in three typical organic solvents, including polyethylene glycol 200 (PEG200), diethylene glycol (DEG), and ethylene glycol (EG). The results showed that high-concentration TETA nonaqueous absorbents demonstrate advantages in absorption rate and regeneration energy consumption. The average absorption rate of 2.0 and 5.0 mol/L TETA/EG was 2.84 and 4.70 times that of 0.6 mol/L, respectively. The energy consumption of TETA/EG and TETA/DEG decreased by 29.4 and 25.6% as the concentration increased from 0.6 to 5.0 mol/L. In addition, the high-concentration TETA/PEG200 absorbent demonstrated observable tolerance for water vapor, which usually exists in flue gas. Results also showed that microwave regeneration was superior to conventional conduction heating especially when high-concentration TETA/PEG200 absorbent were used. The energy consumption of microwave regeneration of the absorbent with a concentration of 0.6, 2.0, and 5.0 mol/L was reduced by 65.9, 81.2, and 86.0%, respectively when compared with conduction heating. © 2022 Society of Chemical Industry and John Wiley & Sons, Ltd.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Yao Liu,Luotian Lv,Han Feng,Hao Liu,Yongqing Wang
Developing highly efficient photocatalysts for CO2 reduction is critical for addressing global warming and energy supply issues. However, both single-component metal-organic frameworks (MOFs) and conventional semiconductor catalysts face significant challenges, such as severe charge recombination, poor CO2 adsorption capacity, and low utilization of solar energy in the photocatalytic reduction of CO2. To address these limitations, the formation of Z-scheme heterojunction photocatalyst has been proved to be an effective way to suppress the recombination of photoinduced carriers. In this work, an indirect Z-scheme heterojunction photocatalytic system, namely, Cu-doped-ZIF-67Co/Bi4O5Br2, is prepared by means of ion-doping and in situ growth strategy. Electrochemical characterization demonstrated the formation of p-type ZIF-67CoCu nanocubes and n-type Bi4O5Br2 nanosheets. The indirect Z-scheme band structure of the heterojunction was well-defined by X-ray photoelectron spectroscopy (XPS), Mott–Schottky test, and ultraviolet photoelectron spectroscopy (UV). The optimal Cu-doping ratio (molar ratio) and composite ratio (mass ratio): 1% ZIF-67CoCu(1:1)/Bi4O5Br2 exhibits excellent photocatalytic CO2 reduction performance, a remarkable rate of 6469.88 μmol·g–1·h–1, and a high CO selectivity of 97%. Compared to individual ZIF-67CoCu and Bi4O5Br2, the performance of reduction of CO2 to CO is improved by 4.19 and 8.64 times, respectively. Density functional theory calculations and in situ diffuse reflectance infrared Fourier transform spectroscopy results had shown that the existence of Cu in ZIF-67 facilitates the desorption of CO and the reduction process features the key CO* intermediate during the photoreduction of CO2 to CO on 1% ZIF-67CoCu/Bi4O5Br2. This study provides an exciting example for the design and understanding of the ion-doped MOFs and the semiconductor construction of indirect Z-scheme photocatalytic system for promoting photocatalytic capacity.
研究领域:
材料科学
·
环境科学
·
化学
·
光催化
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Caifeng Xia,Qikang Yin,Xinle Sun,Qinglong Liu,Sen Liu,Shuxian Wei,Siyuan Liu,Weifeng Lv,Zhaojie Wang,Xiaoqing Lu
As a unique polymer of intrinsic microporosity, PIM-1 has great potential in mixed matrix membranes (MMMs) for gas separation with ultra-high permeability. However, the separation performance, e.g. CO 2 /N 2 separation, is still limited by its poor selectivity. In this work, PIM-1-based MMMs containing tartaric acid anion intercalated layered double hydroxides (TA-LDH) nanofillers are successfully prepared. The uniformly dispersed TA-LDH in the PIM-1 matrix contributes to optimizing the stacking of polymer chains for accessible pores, which is conducive to CO 2 diffusion. In addition, the assistant experiment and theoretical calculation point out that the -COO - , –OH between the TA-LDH layers had an affinity for CO 2 , creating a two-dimensional fast transport channel between the enlarged interlayer space. Compared with the pristine PIM-1 membrane, the CO 2 permeability and CO 2 /N 2 selectivity of 0.7 % TA-LDH/PIM-1 membrane is increased by 43.19 % and 105.48 %. The excellent gas separation performance with CO 2 permeability of 8343.18 Barrer and CO 2 /N 2 selectivity of 39.02 exceeds the 2019 Robson upper limit. This paves a new way to improve the gas separation performance of PIM-1-based MMMs and suggests high perspectives for real applications.
研究领域:
材料科学
·
环境工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Weiyi Chen,Bin Han,Chen Tian,Xueming Liu,Shujie Liang,Hong Deng,Zhang Lin
Reducing carbon dioxide (CO 2 ) to various value-added chemical products by photocatalysis could effectively alleviate the serious problems of global warming and energy shortages. Currently, most commonly prepared photocatalysts present poor performance under visible light irradiation. In this study, we adopted a facile, scalable and controllable approach to prepare ultrathin two-dimensional (2D) porous Co 3 O 4 catalysts (Co 3 O 4 -NS) by air calcining of the ultrathin metal-organic framework (MOFs) nanosheet templates to validly reduce CO 2 with a Ru-based photosensitizer under visible light irradiation. Benefitting from the structural nature of MOFs precursors, the calcined Co 3 O 4 -NS inherit the morphology of 2D and well-developed porosity, which support the transport of electrons, enhance the adsorption of CO 2 molecules, and render abundant catalytic sites for CO 2 activation. As a result, the CO generation rate is approximately 4.52 μmol·h −1 with selectivity of 70.1%, which is superior to the Co 3 O 4 bulk catalysts (Co 3 O 4 -BK). Additionally, density functional theory (DFT) calculations reveal that the model of Co 3 O 4 monolayer has stronger CO 2 adsorption energy than that of the Co 3 O 4 bulk, which is beneficial for the CO 2 -to-CO conversion. This MOF-engaged strategy provides new insight into the controlled synthesis of advanced ultrathin holey nanosheets to improve the efficiency of photocatalytic CO 2 reduction.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Yufang Wu,Zhenqiang Lv,Xin Zhou,Junjie Peng,Yuning Tang,Zhong Li
We report a bifunctional SBU-tuning strategy that simultaneously enhances the selective CO 2 adsorption capacity of Cu-BTC and its structural stability under moisture. A series of Gly@Cu-BTCs were prepared by grafting glycine (Gly) to the secondary building units (SBUs) of the commercially available Cu-BTC through the nano-seed assistant ultrafast room temperature synthesis. N 2 isotherms evidenced higher BET specific surface area and pore volume of Gly@Cu-BTCs than that of Cu-BTC. Hence, Gly 0.3 @Cu-BTC exhibited a superior CO 2 capacity of 5.4 mmol/g at ambient conditions, which is 12% higher than that of Cu-BTC. Besides, the adsorptive selectivity of Gly 0.3 @Cu-BTC for the equimolar CO 2 /CH 4 and CO 2 /N 2 mixtures was separately up to 8.53 and 59.38, being 11% and 15% higher compared to that of Cu-BTC. More importantly, the stability of Gly 0.3 @Cu-BTC against moisture was improved. After 10 days’ exposure in 55% relative humidity, Gly 0.3 @Cu-BTC preserved 80% of its original CO 2 capacity, while only 9% CO 2 capacity remained for Cu-BTC. In addition, negligible CO 2 capacity loss of Gly 0.3 @Cu-BTC was observed in the subsequent 10 days in moisture after the initial exposure. Gly 0.3 @Cu-BTC exhibited excellent regenerability, and its CO 2 desorption efficiency reached up to 98% based on the consecutive adsorption-desorption cycles. The origination of the improved stability under moist of Gly 0.3 @Cu-BTC was interpreted with DFT calculation. The bifunctional SBU-tuning strategy demonstrated in this work enables the potential adsorptive separation application of Cu-BTC under moist working condition.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2023
·
IF 3.7
Zhan-Kuo Guo,Han-Qing Chen,Hui-Lin Jiang,Bao-Xia Dong,Yun-Lei Teng
Storing and hydrogenating CO2 to CH4 is an efficient solution to alleviate the greenhouse effect and energy shortage. This work demonstrated that the CaO-captured CO2 could be selectively converted to CH4 by Ni- and hydrogen-assisted calcium looping (CaL) processes in a batch reactor. The Ni/CaO composite was first synthesized in one step at room temperature by calcium-induced hydrogenation of Ni-mixed calcium carbonate without the use of any solvent and CO2 emission. The CO2 capture properties over the Ni/CaO composite and the methanation properties of the Ni/CaCO3 composite produced after CO2 capture were then studied in a batch reactor. It was proved that the CO2 capture properties of CaO can be improved, the CaO recovering temperature can be significantly lowered, and valuable CH4 can be selectively produced by Ni- and hydrogen-assisted calcium looping processes at moderate/high temperature. The 68.58% methane yield and 100% methane selectivity were achieved under relatively mild conditions. After five Ni- and hydrogen-assisted CaL processes, the methane yield still reaches 45%. This study offers a novel energy-saving CaL process, which can be utilized for facile and selective conversion of the CaO-captured CO2 to CH4.
研究领域:
化学工程
·
环境科学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Desen Zhou,Xuan Zhang,Zheng Li,Jun Zhang,Tielin Wang,Shaowen Cao
Photocatalytic conversion of CO 2 to usable fuels provides a new strategy for solving energy problems and the greenhouse effect. Porphyrin-based metal-organic frameworks (MOFs) are promising in photocatalysis due to their remarkable light harvesting ability, and the metal active site and its coordination environment can be further adjusted to achieve the high activity. In this work, g-C 3 N 4 /PCN-222 composites with different porphyrin metal centers were fabricated and the g-C 3 N 4 /PCN-222(Fe III ) catalyst showed the highest photocatalytic CO 2 reduction performance than that of g-C 3 N 4 /PCN-222(Fe II ) and other g-C 3 N 4 /PCN-222( M , M = Co, Ni, Cu, Zn) composites. Experimental studies and theoretical calculations showed that the axial coordination in g-C 3 N 4 /PCN-222(Fe III ) distorts the square planar field (Fe-N4) to quasi-octahedral coordination, which led to the moderate adsorption ability of CO 2 reduction intermediate (*CO), resulting in the high photocatalytic activity.
研究领域:
材料科学
·
环境科学
·
化学工程
·
催化
✓ 已验证
产品关联
DOI
高影响因子
Frontiers of Environmental Science & Engineering
·
2013
·Vol. 8
·期 2
·162-168
·
IF 0.886
Xie Jiangkun,Yan Naiqiang,Liu Fei,Qu Zan,Yang Shijian,Liu Ping
Porous ZIF-7 with the sodalite (SOD) cage structure (ZIF, Zeolitic imidazolate framework) were synthesized by the solvothermal method. Synthesized material was characterized by powder X-ray diffraction (PXRD), thermal gravity (TG), scanning electron microscopy (SEM) and N 2 adsorption analysis. ZIF-8 with the SOD structure and a little larger pore window was synthesized in a similar way and was characterized for comparisons. Thermal stability and structural stability of ZIF-7 were tested through PXRD analysis, and the capability of the material for CO 2 capture from simulated flue gas was investigated through physical adsorption method. The results showed that CO 2 adsorption capacity on ZIF-7 was about 48 mL·g −1 while the capacity on ZIF-8 was about 18 mg·g −1 (at 12°C and 0.98 P / P
0 relative pressure). Furthermore, the impact of flue gas components on adsorption capacity of ZIF-7 and the selectivity of CO 2 against N 2 on ZIF-7 was also investigated in this work.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 46
·期 5
·2189-2197
·
IF 3.591
Yangyang Xin,Dechao Wang,Dongdong Yao,Hailong Ning,Xiaoqian Li,Xiaoqian Ju,Yichi Zhang,Zhiyuan Yang,Yahong Xu,Yaping Zheng
Porous liquids (PLs), a new class of materials with permanent pores and macroscopic flowing behaviors, have attracted much attention for CO2 capture. However, the preparation of PLs is always complicated, which is not suitable for the scale-up. Herein, we propose a rather simple and feasible strategy based on post-synthetic modification of pore generators and the like-dissolves-like principle to synthesize UiO-66-PLs with low-viscosity. To be specific, the metal–organic framework (MOF) UiO-66 with hydroxyl groups (denoted UiO-66-OH) was modified by an organosilane (denoted KH550 or SID) via a post-synthetic modification method, obtaining the pore generator UiO-66-OS (denoted UiO-66-KH550 or UiO-66-SID). Then, the UiO-66-OS was dispersed into two different sterically hindered polydimethylsiloxane solvents (PDMS400 or PDMS6000). Thereby, a series of type 3 PLs (UiO-66-PLs) with superior fluidity at room temperature and accessible porosity were obtained. For instance, the viscosities of UiO-66-KH550-PDMS400 and UiO-66-SID-PDMS400 were 1.1 and 1.5 Pa S at 25 °C, respectively, which were far lower than those of values reported thus far. In addition, gas sorption–desorption measurements indicated that the UiO-66-PLs exhibit superior CO2 sorption performance and great potential for CO2/N2 separation. Moreover, molecular simulation was carried out to verify the retained accessible porosity. Notably, the strategy of constructing type 3 PLs based on the post-synthetic modification of MOFs with organosilane and the like-dissolves-like principle not only provides a new solution for the development of low-viscosity PLs, but also opens a new path for the construction of other types of advanced porous material (APM)-based (e.g., covalent organic frameworks (COFs), porous organic cages (POCs)) PLs, which have potential applications in the fields of gas trapping storage, and catalysis.
研究领域:
材料科学
·
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Guangmin Ren,Sitong Liu,Xiangchao Meng
This paper reports on a Bi2MoxW1–xO6 solid solution with excellent photocatalytic activity in CO2 reduction. Under simulated sunlight, the Bi2Mo0.25W0.75O6 solid solution achieved a CO generation yield of ≤298.2 μmol g–1 over 3 h, which was 2.1 and 1.5 times larger than those of pristine Bi2WO6 and Bi2MoO6, respectively. Via an in-depth study of the mechanism, this excellent photocatalytic activity was determinied to be probably due to two major contributions: (1) the formation of oxygen vacancies on the Bi2Mo0.25W0.75O6 solid solution, which provided more reactive sites for adsorption and activation of CO2, and (2) modulation of the electronic band structure, which facilitated charge separation. Mechanistic and reaction pathways have been deeply explored and proposed.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
DOI
PubMed
高影响因子
Advanced Science
·
2025
·
IF 14.1
Fengyi Zhong,Jianping Sheng,Chenyu Du,Ye He,Fengying Zhang,Yanjuan Sun,Ying Zhou,Fan Dong
Heterojunctions, known for their decent separation of photo-generated electrons and holes, are promising for photocatalytic CO 2 reduction. However, a significant obstacle in traditional post-assembled heterojunctions is the high interfacial barrier for charge transfer caused by atomic lattice mismatch at multiphase interfaces. Here, as research prototypes, the study creates a lattice-matched co-atomic interface within CsPbBr 3 -CsPb 2 Br 5 polytypic nanocrystals (113-125 PNs) through the proposed in situ hybrid strategy to elucidate the underlying charge transfer mechanism within this unique interface. Compared to CsPbBr 3 nanocrystals, the 113–125 PNs exhibit a remarkable 3.6-fold increase in photocatalytic CO 2 reduction activity (173.3 µmol −1 g −1 within 5 h). Furthermore, Kelvin probe force microscopy results reveal an increase in the built-in electric field within this lattice-matched co-atomic interface from 43.5 to 68.7 mV, providing a stronger driving force for charge separation and directional migration. Additionally, ultrafast transient absorption spectroscopy uncovers the additional charge carrier transfer pathways across this lattice-matched co-atomic interface. Thus, this unique co-atomic interface significantly promotes the interfacial electronic coupling and mitigates the charge transfer barrier, thus facilitating efficient charge separation and transfer. These insights underscore the importance of interfacial structure in heterojunction design and comprehending the intricate interplay between interface and carrier dynamics.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Mengchen Wu,Yang Yang,Jing Zhao,Rui Liu
In CO 2 electroreduction, mutative intermediates and the challenging C C coupling necessitate the spatial interplay between active sites and through dynamically optimizing configurations. Herein, we anchor ethylenediaminetetraacetic acid (EDTA)-bonded Cu x+ /Bi 3+ pair within UiO-66 for a spontaneous spatial-optimizing CO 2 -to-C 2 H 4 electroreduction. Ab initio molecular dynamic (AIMD) simulation visualizes that such metal pair adaptively interacts with intermediates. Density functional theory (DFT) elicits the componential synergy, in which an upshift d-band of Cu activates CO 2 being protonated into *COOH while Bi site stabilizes oxygenated dimers for deep hydrogenation. The dynamic feature of such pair affords large freedom for sorption and migration of various intermediates, which consequently bestows UiO-66-EDTA/CuBi a maximal FE C 2 H 4 of 47 % and a total current density over 100 mA cm −2 in the flow cell.
研究领域:
材料科学
·
催化化学
·
能源转化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）