JOURNAL OF POROUS MATERIALS
·
2023
·
IF 2.6
Liu Hai,Song Tao,Wang Yimin,Zhang Xiaoli,Cui Li,Liu Tianxia,Yuan Zhen
Electrocatalysis serves as a highly effective approach to both mitigate greenhouse gas emissions and produce high-value chemicals. Copper-based catalysts have garnered considerable attention due to their immense potential in this domain. Improving the selectivity and activity through optimizing preparation strategies is of paramount importance. In this study, the mechanochemical method was first used for preparing copper-based composite metallic oxide electrocatalysts. Spherical CuO, Sn-CuO, and Sn-In-CuO catalysts were prepared, and their electrochemical CO 2 performance was evaluated. Among them, the Sn-In-CuO catalyst demonstrated the best performance in reducing CO 2 to CO products. Within the potential range of −0.6 V to −1.1 V vs. RHE, the Faradaic efficiency of the CO product was consistently above 93.56%, with a maximum Faradaic efficiency of 96.11% achieved at −0.9 V vs. RHE. Sn-In-CuO also exhibits good stability with high Faradaic efficiency of CO above 87.97% for a duration of 6 h under the potential of −0.6 V vs. RHE in a 0.1 M KHCO 3 electrolyte. The excellent performance is speculated to be attributed to the generation of a large number of defects and the introduction of metal doping, which increases the number of active sites through the mechanochemical method.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Qiang Sun,Jia Xiong,Hongxia Gao,Wilfred Olson,Zhiwu Liang
Catalytic CO 2 desorption from rich amine solution is a practical approach to reducing energy consumption for amine regeneration. In this study, for the first time, the catalytic effect of environmentally friendly, imidazole series ionic liquids ([Bmim]PF 6 , [Bmim]BF 4 , [Bmim]HSO 4 , [Bmim]NO 3 , [Bmim]CH 3 COOH, [Bmim]Cl, [Bmim]Br, and [Bmim]I) is evaluated in terms of CO 2 desorption rate, amount of CO 2 released, and heat duty. Overall, the [Bmim]PF 6 catalyst shows excellent catalytic activity for CO 2 desorption, increasing the quantity of CO 2 released by 21.35% and reducing the relative heat duty by 17.59%. In addition, the catalytic applicability of [Bmim]PF 6 for secondary and tertiary amine systems was evaluated. Of note, the homogeneous [Bmim]PF 6 catalyst presents good stability during 5 cycles. The catalyst/MEA (monoethanolamine) solution ratio of 3 wt% retained about 94% of the catalytic performance after five cycling tests without any reactivation step, showing the potential application of this desorption technology for CO 2 capture with lower heat duty.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Shanlong An,Xin Huang,Nuo Li,Qiangwei Li,Tieyue Qi,Rujie Wang,Lidong Wang
2-amino-2-methyl-1-propanol (AMP) combines the advantages of the faster reaction rate of primary/secondary amines and the high absorption capacity of tertiary amines, making it a highly promising alternative to monoethanolamine (MEA). However, at high AMP concentrations, the absorption products are prone to solid crystallization, resulting in unstable operation of the carbon capture system. In this work, by adding a small amount of diethylenetriamine (DETA) to AMP, the crystallization of reaction products can be effectively controlled and AMP-DETA absorbent possesses a high absorption rate, low regeneration energy, and low metal corrosion rate. Wetted-wall column tests were performed to comprehensively evaluate the mass transfer kinetics and the effect of crucial conditions, and the diffusion coefficient, gas–liquid mass transfer coefficient, enhancement factor, and mass transfer resistance distribution were obtained. The effect of the addition of DETA on the solubility of HCO 3 − was verified. DETA carbamate was more likely to form intermolecular hydrogen bonds with HCO 3 − , thus reducing the formation of dimeric or multichain macromolecules between HCO 3 − molecules through hydrogen bonds and inhibiting the crystallization of high concentration HCO 3 − . HCO 3 − can accelerate the desorption rate by participating in the deprotonation of protonation amines. The results demonstrated that the average regeneration energy of the AMP–DETA absorption system was reduced by 21.2 % relative to that of 5 M MEA, and its metal corrosion rate was 0.07 mm/a, which was only 7.9 % of MEA under the same conditions. The results contribute to the industrial application of AMP–DETA.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Haiqiang Mu,Yu-An Li,Xiuli Wang,Feng Li,Xin Du,Jing Li
The rational modulation of the coordination environment of the active center of single-atom catalysts (SACs) is a potential strategy to improve the activity and selectivity of electrocatalytic CO 2 reduction. We developed a series of single-atom Ag-anchored on N -doped carbon catalysts with different N -coordination environments by regulating the carbon source (glucose/graphene oxide, GO). Results demonstrated that the CO 2 -to-CO/C 2 H 5 OH pathway can be converted through reasonable regulation of the content of pyrrolic N and pyridine N. At a highly dominant pyrrolic N content of 40.0 %, the electrocatalyst of Ag-N-rGO 0.025 M facilitates the formation of CO with a Faradaic efficiency (FE) of 69.7 %. By contrast, when the pyridine N content is 70.5 %, the best Ag-N-C 0.05 M catalyst in the H-cell shows an FE of 42 % for C 2 H 5 OH at −0.97 V vs. RHE; moreover, the FE is stable at 40 % within 31 h. Density functional theory calculations further confirm that the pyrrolic N site is conducive to the conversion of CO 2 to intermediate *CO, whereas pyridine N exhibits the highest binding energy (ΔG = -4.73 eV) to hold *CO intermediates for dimerization, consequently steering the pathway to the formation of C 2 H 5 OH. The results of this study provide novel insights into the rational design of carbon-based SACs based on efficient electrochemical CO 2 reduction reaction and the regulation of CO 2 selectivity and activity for C 2 H 5 OH production.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Yuliang Li,Guojie Zhang,Chenlei Wu,Jun Liu,Guoqaing Li,Ying Wang,Yuqiong Zhao
Low-cost nitrogen-enriched activated carbons (PNACs) with high microporosity were prepared by a simple one-step activation doping process using KOH as a chemical activator and melamine formaldehyde (MF) as a nitrogen source. These PNACs have shown great potential as effective CO 2 adsorbents. The resulting PNACs were mainly microporous structure, with surface areas ranging from 736 to 2144 m 2 /g and total pore volumes ranging from 0.565 to 1.366 cm 3 /g. The CO 2 adsorption capacities of PNACs were in the range of 2.53-6.07 mmol/g and 1.59–4.13 mmol/g at 0 °C and 25 °C under 1 bar, respectively. Additionally, the CO 2 /N 2 selectivity of the PNACs ranges from 11.15 to 26.86 at a CO 2 partial pressure of 0.1 bar. The experimental isotherm data were analyzed using various equations and the Toth isotherm equation was found to be the most accurate mathematical model to describe the CO 2 adsorption isotherm of the activated carbon. This result further confirms that PNACs have a non-homogeneous pore structure. The exceptional CO 2 adsorption properties can be attributed to the high microporosity and nitrogen content of the PNACs. The relationship between the physicochemical properties and CO 2 adsorption performance of the activated carbon was further investigated by relevance analysis. At 0 °C and 1 bar, it was observed that the pore structure played a predominant role in the CO 2 adsorption process of PNACs. During this condition, PNACs mainly exhibited physical adsorption, which was primarily governed by the microporous filling mechanism. However, at 25 °C and 1 bar, both microporosity and nitrogen content contribute equally to the CO 2 adsorption effect. This observation confirms that the pore structure and nitrogen functional groups work synergistically to influence the CO 2 adsorption performance of PNACs. The adsorption mechanism of PNACs can be described as physical adsorption, driven by the cooperation between nitrogen functional groups and the filling of micropores. This innovative one-step activation doping process successfully converts agricultural and plastic waste into sustainable and high-performance CO 2 adsorbents. It provides new insights for mitigating the greenhouse effect and addressing the issue of plastic pollution .
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2023
·
IF 6
Yuting Wang,Xiaoyu Wang,Liming Chai,Enna Wang,Xionghui Wei,Zhaojun Wu,Jianbin Zhang
Density ( ρ ) and viscosity ( η ) data of polyethylene glycol 300 (PEG300) + N-methyldiethanolamine (MDEA) binary system at T = (298.15–318.15) K with a step of 5 K were measured at P = 1005 hPa. After that, the experimental ρ and η values were correlated and predicted by several semi-empirical models. Meanwhile, the Jouyban-Acree model presented a better fitting for the density, and the McAllister four-body equation presented a better fitting for the kinematic viscosity. Based on the ρ and η values, excess molar volume ( V m E ), partial molar volume ( V 1 ¯ and V 2 ¯ ), viscosity deviation ( Δη ), and excess Gibbs energy of activation of viscous flow ( Δ G ∗ E ) of PEG300 (1) + MDEA (2) binary system were systematically calculated and analyzed. These excess properties showed the predominance of intermolecular self-conjugation in PEG300 (1) + MDEA (2) binary system, and it was further demonstrated by various spectral characterizations. Importantly, the PEG300 + MDEA aqueous system was used for 5 CO 2 absorption (room temperature)-desorption (371.15 K) cycles at a CO 2 flow rate of 200 mL/min, with the average CO 2 capture performance of 0.65 mol CO 2 /mol MDEA of per cycle, demonstrating excellent absorption capability, and remained stable throughout the entire cycle.
✓ 已验证
产品关联
DOI
高影响因子
Nano Energy
·
2023
·
IF 17.6
Hao Zhang,Ying Wang.,Qiong Lei,Ying Wang,Chiu Tang,Jun Yin,Tsz Woon Benedict Lo
Tracking the evolution of electrocatalysts over oxide-derived Cu materials during the electrochemical CO 2 reduction reaction (eCO 2 RR) is pivotal for optimizing the product selectivity toward desired multi-carbon (C 2+ ) products. However, the identification of the true intermediate active catalyst is still unclear. Here, we adopted a multi-modal characterization approach, primarily based on operando powder X-ray diffraction and operando micro-Raman spectroscopy, to study three Cu 2 O precursors with different morphologies, namely, octahedral (O-), cubic (C-), and nanowire (N-Cu 2 O). This multi-modal approach allows us to investigate the Cu 2 O nano-crystallites from the interface to the bulk structure. The results suggested notably different electrochemical reduction kinetics. 26.1% O-Cu 2 O and 90.6% C-Cu 2 O were reduced to much smaller Cu(0) domains after two hours of time-on-stream; N-Cu 2 O, with notably higher surface-to-volume ratio, was completely reduced within 45 min of time-on-stream. We accordingly observed a structure-reactivity correlation where a more intricate Cu 2 O/Cu grain network (and hence Cu + -Cu 0 junctions) as observed in O-Cu 2 O, can lead to stable and quantitative production of ethylene at the Faradic efficiency of around 40% (in stark contrast to those of C- and N-Cu 2 O). The synergy between the Cu 2 O and Cu phases was also verified by density functional theory calculations. The upshifted d -band center of Cu 2 O/Cu in O-Cu 2 O is the most conducive toward the production of ethylene, whereas the downshifted d -band center of Cu 2 O/Cu in C-Cu 2 O leads to a decreased production of ethylene in the expense of unwanted production of hydrogen. We envisage that system optimization and design of new catalysts will become more facile and efficient using a related multi-modal operando characterization philosophy.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Su Dan Bao,Wei Jian,Jin Hao Li,Yong Sheng Bao,Agula Bao
Due to their outstanding physicochemical characteristics, heteroatom-doped porous carbon materials have attracted significant attention. Herein, the pore structure and N content of the NPC-X material were regulated via P doping using a simple pyrolysis and activation method. The CO 2 adsorption mechanism and electronic properties of the materials were determined by combining characterization results and theoretical calculations. Density functional theory calculations show that P has the capability to increase the porosity and facilitate the generation of pyridine-N and pyrrole-N functional groups in N-doped carbon materials. Moreover, the interaction between N groups and CO 2 can be effectively elucidated through the analytical density of states. The experimental results show that the NPC-2 sample exhibits excellent CO 2 adsorption performance (4.50 mmol/g at 298 K and 1 bar) and recycling stability. This study presents new synthetic approaches for the preparing N/P codoped carbon materials and explores the CO 2 adsorption mechanism of materials with multiple coexisting functionalities.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Zeyu Cao,Jingfeng Li,Xinai Zhang,Bo Zhang,Jinchao Li,Yaping Zhang,Qingchun Zhang,Ping Zhang,Yingze Song
Designing and synthesising electrocatalysts with low overpotential, high activity, selectivity, and stability for the CO 2 reduction reaction (CO 2 RR) is crucial for addressing environmental challenges and realising the artificial carbon cycle. In this study, we successfully synthesised a nitrogen-doped carbon-supported diatomic electrocatalyst comprising atomically dispersed CuN 4 and NiN 4 bimetallic centers. This was confirmed through extensive characterisation using high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption spectroscopy techniques. The as-synthesised CBN-CuNi electrocatalyst exhibited exceptional selectivity and stability in CO 2 RR. Over a wide potential range from − 0.60 to − 1.10 V vs RHE, CBN-CuNi maintained over 90% Faraday efficiency for CO (FE CO ) production. Notably, at − 0.9 V vs RHE, it achieved a remarkable selectivity with a maximum FE CO of 97.9%, surpassing single metal catalysts, including CBN-Ni and CBN-Cu. Furthermore, CBN-CuNi demonstrated outstanding stability, sustaining over 90% FE CO production for 40 h of continuous electrolysis, surpassing many existing electrocatalysts. These findings highlight the potential of the as-synthesised bimetallic electrocatalyst CBN-CuNi in the electrochemical reduction of CO 2 to CO, contributing to advancing the artificial carbon cycle and addressing environmental concerns.
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Juan Yang,Xiang Liu,Kexin Song,Xinyue Li,Dihua Wang
Understanding of the correlation between physico-chemical property of adsorbent and the adsorption performance of contaminant is very significant for developing high-efficient materials to remove antibiotic contamination from water. In this work, a novel kind of carbon adsorbent (EC) derived from CO 2 and activated ECs with modified structure via a facile chemical method using H 2 and KOH were prepared. The synthetic carbon materials (EC, EC-H 2 , and EC-KOH) were then applied to remove tetracycline (TC). The kinetics of adsorption for these three carbon materials all well fitted the pseudo-second-order kinetic model. The experimental data of adsorption isotherm had good compatibility with Langmuir and Freundlich models (R 2 > 0.90), but the Temkin model was the most applicable for all adsorbents (R 2 > 0.98). A super-high adsorption capacity of EC-KOH obtained from Langmuir fitting was 933.56 mg g −1 , which was much higher than that of EC-H 2 (538.91 mg g −1 ) and EC (423.30 mg g −1 ), possibly due to its larger specific surface area (S BET ), pore volume, and specific surface chemical structure. Moreover, it was found that surface functional groups and large aperture of adsorbents had a positive effect on adsorption rate. More adsorption sites and surface functional groups of adsorbents were beneficial to enhance the adsorption affinity. These results are of great benefit to the directional control of carbon structure to increase the adsorption performance in rate, capacity, and affinity of antibiotics.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Songcai Cai,Jing Chen,Qiang Li,Hongpeng Jia
CO2 conversion into chemical fuels is a sustainable approach to the concurrent mitigation of the energy crisis and the greenhouse effect. It is still urgently desirable but quite challenging to explore a promising catalyst for CO2 photoreduction due to the severity in the fast recombination of electron holes and the deficiency of active sites, which have a tremendous influence on the catalytic behavior. In this regard, mesoporous TiO2 nanospheres containing oxygen vacancies (OVs) and metallic Au nanoparticles (NPs) were successfully prepared and showed markedly enhanced CO2 reduction activity and CH4 selectivity by the simple combination of photocatalysis with the simultaneous photothermal effect under full-spectrum irradiation. The dual introduction of OVs and a Au/TiO2 Schottky junction can not only serve as an electron sink to significantly improve the charge separation/transfer efficiency but also show effective photothermal conversion to raise the local temperature of the catalyst, thus resulting in an enhanced shuttle of electrons and desorption of products. This study not only offers new insights into the integrated tuning of charge recombination processes but also demonstrates that the photothermocatalysis has great potential in CO2 reduction.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2021
·
IF 13.084
Chenyang Shen,Kaihang Sun,Zhitao Zhang,Ning Rui,Xinyu Jia,Donghai Mei,Chang-jun Liu
Iridium (Ir) catalysts have been extensively applied in homogeneous and photocatalytic CO2 conversion. However, CO2 hydrogenation to methanol over the supported Ir catalyst in a heterogeneous flowing reactor has not been reported yet. Here, we report that indium oxide supported Ir catalyst (Ir/In2O3) of high dispersion is very active for CO2 hydrogenation to methanol. Compared to In2O3, Ir/In2O3 shows a significantly higher activity with even higher methanol selectivity. For example, CO2 conversion of 17.7% is achieved on Ir/In2O3 of 10 wt % Ir loading with methanol selectivity over 70% and high methanol space time yield of 0.765 gMeOH h–1 gcat–1 at 4/1 of the CO2/H2 feed ratio, 21 000 h–1, 300 °C, and 5 MPa. With the catalysts tested, the higher Ir loading causes the higher activity. The catalyst characterization confirms an intense interaction between iridium and In2O3, which causes the high dispersion of the Ir catalyst with the Ir–In2O3 interface as the active site for selective hydrogenation of CO2 into methanol. The Ir loading not only enhances the formation of oxygen vacancies but also stabilizes the vacancies for improved CO2 activation. Further density functional theory studies reveal that the reverse water–gas shift route is more favorable over the formate route for CO2 hydrogenation to methanol over Ir/In2O3 catalyst.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）