Energy Technology
·
2025
·
IF 3.6
Hui Huang,Qi Xu,Liangyun Yu,Lidong Li,Ying Zhang,Fennv Han,Qi Zhang
Currently, there is a thermodynamic and kinetic mismatch between carbon dioxide methanation. Carbon dioxide is stable in nature and requires a highly active catalyst to facilitate its reduction reaction. In this article, Ru/ZrO 2 catalysts are prepared by a structure-directed derivatization strategy using zirconium-based metal-organic frameworks (MOFs) (UiO-66) as precursors. The porous framework structure of MOFs was utilized to construct Ru nanoparticles with a large size (≈9.7 nm). Photothermal catalysis is employed, and the photoexcitation induced the transfer of electrons from the conduction band of ZrO 2 to Ru, which elevated the electron density of Ru to the enriched state and promoted the activation of CO 2 adsorption, while the photothermal effect facilitated the warming of the catalyst bureau, which provided a favorable condition for CO 2 methanation. The compositional valence, morphology, specific surface area, bandgap and other properties of the catalysts were evaluated by X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscpe, Brunner-Emmet-Teller measurements, hydrogen temperature-programmed reduction, CO 2 -TPD, ultraviolet–visible, photoluminescence, and photocurrent response characterization. The experimental results showed that 99% methane selectivity and 120.354 mmol g cat −1 h −1 methane yield were achieved at 1 MPa and photothermal (250 °C) conditions.
✓ 已验证
产品关联
DOI
高影响因子
Chemical Science
·
2025
·
IF 7.4
Jiye Feng,Danni Shi,Fei Wang,Yiming Zou,Weicheng Li,Wenbiao Zhang,Huai-Jun Lin,Yuying Meng,Qingsheng Gao
The electrochemical reconstruction of metal-organic frameworks (MOFs) offers a promising approach for in situ fabrication of high-performance electrocatalysts. However, this innovation is often hindered by unpredictable structural transformations due to the complex thermodynamic and kinetic interplay of such multiple electrochemical and chemical processes. Herein, the reaction-atmosphere (Ar or CO2) guided reconstruction of Cu-based MOFs to Cu nanoparticles with mix-valence surface/interfaces was for the first time investigated to unravel the kinetic contribution made by intermediate chemisorption. As shown, Cu-1,3,5-benzenetricarboxylate (HKUST-1) with frangible Cu-O4 nodes undergoes thermodynamically favored reduction quickly upon applying cathodic potentials, followed by the varied surface changes kinetically governed by the intermediates of hydrogen evolution or CO2 reduction reactions (HER or CO2RR). Under an Ar atmosphere, the predominant HER increases the [OH-] of the microenvironment near cathodes and thereby boosts the re-oxidation of in-situ formed Cu toward Cu/Cu2O interfaces. Conversely, the CO2RR facilitates the strong adsorption of *CO on Cu surfaces, effectively preserving Cu(0) species. Thanks to the rich Cu/Cu2O interfaces with the lowered energy barrier for *CO-*CO coupling during the subsequent CO2RR test, the restructured electrocatalysts under Ar affords the obviously improved CO2-to-C2H4 conversion as compared with the counterpart restructured under CO2. Such atmosphere-controlled reconstruction strategy is further validated using CuBDC (BDC = 1,4-benzenedicarboxylate) with labile Cu-O4 nodes, while CuPz2 (Pz = pyrazole) with robust Cu-N4 coordination remains stable, highlighting the framework-dependent nature. These findings establish atmosphere-controlled reconstruction of metastable MOFs as a powerful tool for rational electrocatalyst design.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Omega
·
2022
·
IF 4.132
Shengyou Shi,Shuie Li,Xiangwei Liu
Deep eutectic solvents (DESs) are a new class of green solvents that exhibit unique properties in various process applications. In this regard, this study evaluated imidazole-type DESs as solvents for carbon dioxide (CO2) capture. A series of imidazole-type DESs with different ratios was prepared through one-step synthesis. The absorption capacity of CO2 in imidazole-type DESs was measured through weighing, and the effects of temperature, hydrogen bond acceptors, hydrogen bond donors, and water content were discussed. DESs absorbed the effects of CO2. Im-MEA (1:2) was selected to linearly fit lnη and 1/T using the Arrhenius equation under variable temperature conditions, and a good linear relationship was found. The results show the best absorption effect for Im-MEA (1:4). At 303.15 K and 0.1 MPa, the absorption capacity of Im-MEA (1:4) was as high as 0.323 g CO2/g DES; through five times of absorption–desorption after the cycle, the absorption capacity of DES was almost unchanged. Finally, the mechanism of CO2 absorption was studied using Fourier transform infrared and nuclear magnetic resonance spectroscopy. The absorption mechanism of imidazole-type DESs synthesized using imidazole salt and an amine-based solution was chemical absorption, and the reaction formed carbamate (−NHCOO) to absorb CO2.
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF CLUSTER SCIENCE
·
2019
·Vol. 31
·期 2
·513-522
·
IF 2.125
Liu Qiang,Liu Yuqi,Zhang Qingqing,Wang Xinying,Li Wei
A new Pr(III)-based metal organic framework with formula {[Pr 2 (C 8 H 3 O 6 N)(SO 4 ) 2 ]·5H 2 O} n was hydrothermally synthesized and characterized by techniques of single crystal X-ray diffraction, infrared spectra (IR), thermogravimetric analysis (TGA), elemental analysis, powder X-ray diffraction (PXRD), and luminescent measurements. X-ray crystal structure analyses reveal that complex 1 is binuclear structure and all Pr(III) atoms show a coordination number of nine with a tricapped trigonal prismatic coordination geometry. Throughout the molecular structure, this lanthanide metal–organic frameworks exhibits a 3D architecture built by the 1D double-stranded chains of Pr ions linked by the 5-nitroisophthalic acid ligand and 2D Pr–SO 4 2− grid. In addition, the fluorescence, nitrogen adsorption properties and carbon dioxide adsorption properties of complex 1 were also investigated. The results indicate that the complex is not only a luminescent and mesoporous material, but also a potential material for selective absorption of carbon dioxide.
✓ 已验证
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Xiaohe Wang,Hongwei Chen,Maosheng Zhang,Chaoran Wang,Yufei Wang,Pu Bai,Libo Li,Wenfu Yan
Silicoaluminophosphate (SAPO) zeolites as one of the most important members of zeolitic materials, providing equally high adsorption capacity of CO 2 as aluminosilicate zeolites, can be used as promising candidate materials for selective adsorption and separation of CO 2 . In this work, desirable from both economic and environmental viewpoints, a green and cost-effective one step synthesis strategy of K-SAPO-34 zeolite was developed in a wholly inorganic system under hydrothermal conditions. The pure K-SAPO-34 crystals can be obtained in a wide range of initial gel compositions. The as-synthesized K-SAPO-34 has high proportion of framework Si (Si / (Si + Al + P) = 0.37) and framework charge density ((Al – P) / (Si + Al + P) = 0.36). Because the presence of silica islands in K-SAPO-34 framework leads to a decrease in the number of extra framework cations per unit cell, the K-SAPO-34 in this work has a high CO 2 adsorption capacity (64.1 cm 3 /g) than the conventional K-SAPO-34 prepared by ion-exchange (1.9 cm 3 /g). Moreover, the K-SAPO-34 in this work has a superior separation performance for CO 2 /N 2 and CO 2 /CH 4 .
✓ 已验证
DOI
高影响因子
Catalysts
·
2023
·Vol. 13
·期 5
·857
·
IF 3.9
Qianqian Zhou,Yanxin Chen,Haoyan Shi,Rui Chen,Minghao Ji,Kexian Li,Hailong Wang,Xia Jiang,Canzhong Lu
Cu2O is a p-type direct bandgap semiconductor with a band gap of 2~2.2 eV, which has excellent visible light absorption and utilization. However, slow charge transfer and poor stability hinder its practical application. In this paper, a facile electrodeposition approach successfully synthesized the heterostructure of p-Cu2O and n-Cu2O. The protective layer of n-Cu2O on the surface of p-Cu2O nanoparticles forms a p/n heterojunction. Due to the p/n heterojunction, the PEC performance of p/n-Cu2O is enhanced significantly. The charge separation efficiency of photogenerated electron/hole pairs in p/n-Cu2O is greatly improved. Therefore, p/n-Cu2O shows superior photoelectrochemical (PEC) CO2reduction reaction (CO2RR) efficiency when used as a photocathode.Keywords:Cu2O;electrodeposition;p/n heterojunction;carbon dioxide reduction reaction
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Xiaoqian Zhang,Chengli Jiao,Xinxin Li,Xiangju Song,Tatiana V. Plisko,Alexandr V. Bildyukevich,Heqing Jiang
Polyamide membrane, fabricated via interfacial polymerization process, is a typical class of facilitated transport membrane for CO 2 separation with amino groups serving as reactive CO 2 carriers. Herein, to further enhance the CO 2 -facilitated transport effect of polyamide membrane, Zn(NO 3 ) 2 is directly introduced into aqueous triethylenetetramine phase for constructing Zn-N coordination polyamide membrane taking advantage of the coordination interaction between Zn ions and amino groups from triethylenetetramine. The good solubility of Zn(NO 3 ) 2 in aqueous amine solution and moderate coordinative ability of Zn ions are beneficial to a uniform distribution of Zn in polyamide layer. The coordination of N from triethylenetetramine monomer to Zn ion centre produces more tertiary amino groups and free amino groups with stronger affinity to CO 2 in Zn-N coordination membrane for enhancing the facilitated transport effect. Additionally, the Zn-N coordination interaction generates smoother surface of membranes when sufficient Zn ions are introduced. The membrane with 0.1 wt% of Zn ions in aqueous phase exhibits the highest CO 2 /N 2 and CO 2 /CH 4 selectivity of 106.7 and 55.2, which increase, respectively, by 75.2% and 99.3% without compromising CO 2 permeance in contrast with pristine polyamide membrane.
✓ 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.
✓ 已验证
DOI
PubMed
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.
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Bao Liu,Chao Cai,Baopeng Yang,Kejun Chen,Yan Long,Qiyou Wang,Shuandi Wang,Guozhu Chen,Hongmei Li,Junhua Hu,Junwei Fu,Min Liu
Electrochemical carbon dioxide (CO 2 ) reduction reaction (CO 2 RR) to obtain C2/multi-carbon fuels is an appealing technology to reduce carbon emission and store intermittent renewable electricity. The C–C coupling process, as the most critical step for generating C2/multi-carbon fuels, strongly depends on the concentration of *CO intermediates around the active sites. In this work, we prepared porous copper nanospheres (P-Cu) that greatly improved the C–C coupling process by enriching *CO intermediates in the pore structure . The specific pore features of P-Cu were characterized in detail by scanning electron microscopy (SEM), transmission electron microscopy (TEM), and nitrogen adsorption/desorption tests. Obviously, the P-Cu exhibits higher specific surface area and richer pore structure than the control sample compact copper nanosphere (C-Cu). The CO gas sensor and temperature programmed desorption (TPD) tests prove that the P-Cu has better CO adsorption and enrichment capacity than C-Cu due to the rich pore structure. As a result, P-Cu exhibited a high C2 selectivity with a Faradaic efficiency (FE C2 ) of 57.22% at −1.3 V ( vs . RHE), which is about 2.5-fold than the C-Cu (FE C2 of 22.71%). This work provides an effective strategy to improve the activity and selectivity of C2 products in CO 2 RR by optimizing the adsorption/enrichment property of intermediates.
✓ 已验证
DOI
高影响因子
ENERGY
·
2022
·
IF 8.857
Yudong Ding,Lijiao Ma,Fengqi Zeng,Xingxing Zhao,Hong Wang,Xun Zhu,Qiang Liao
As a promising CO 2 adsorbent, Aluminum Fumarate (AlFu) metal organic frameworks (MOFs) were explored for pelletizing technology and CO 2 adsorption characteristics. The effects of binder type (sodium carboxymethylcellulose (CMC), aluminum sol (AS)) and content (2.5 wt%-20 wt%), CO 2 partial pressure (0.3 bar–1 bar) and temperature (35 °C–65 °C) on the mechanical performance and adsorption process were investigated. The results revealed that with the increase of binder mass, the pellet mechanical strength rose while the CO 2 adsorption amount decreased. The AlFu pellet with 2.5 wt% CMC could retain the powder porosity and adsorption capacity . The mechanical strength of AlFu@CMC-2.5 wt% achieved 1.486 MPa, and the maximum adsorption capacity was 1.26 mmol/g at 35 °C and 1.0 bar. The CO 2 adsorption capacity was increased with lower adsorption temperature and higher CO 2 partial pressure. Compared with pseudo second order model and pseudo first order kinetic model , Avrami kinetic model could better describe the CO 2 adsorption behavior of AlFu pellet. It indicated that the adsorption process was not a single physical or chemical adsorption . The rate-limiting kinetic analysis showed that the CO 2 adsorption rate was determined by film diffusion and intraparticle diffusion rather than inter-particle diffusion.
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Yifei Ye,Lin Liang,Xiao Zhang,Jianmin Sun
In this paper, a novel arginine-glucose derived carbonaceous-material-loaded SiO 2 composite catalyst (Ar-G-CM/SiO 2 ) was synthesized from non-toxic and harmless reagents (arginine, glucose and tetraethylorthosilicate) by simple hydrothermal process. Mesoporous SiO 2 with high specific area served as support for carbonaceous material and provided extra hydrogen bond donor (HBD) groups. Ar-G-CM/SiO 2 with acid-base dual functional groups ( COOH, NH 2 ) and HBD group ( OH) presented 62% yield and 99% selectivity to product of propylene carbonate in CO 2 cycloaddition reaction with propylene oxide even at 40 °C, 2 MPa under metal-absent and solvent-free conditions. For some less active epoxides with steric hindrance, Ar-G-CM/SiO 2 also showed good yield and selectivity over 90% by raising temperature to 120 °C. Furthermore, the Ar-G-CM/SiO 2 catalyst could be reused for six successive cycles without significant decrease in catalytic activity or structural deterioration, because the carbon deposition was restrained owing to the mesoporous structure of the catalyst.
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）