Catalysts
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2024
·Vol. 14
·期 6
·335
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IF 3.8
Peng Jiang,Yang Yu,Kun Wang,Wenrui Liu
Excessive emissions of carbon dioxide have led to the greenhouse effect and global warming. Reducing carbon dioxide into high-value-added chemicals through solar energy is a promising approach. Herein, a g-C3N4/TiO2heterojunction photocatalyst with efficient electron transfer is designed for photocatalytic CO2reduction. The CH4(18.32 µmol·h−1·g−1) and CO (25.35 µmol·h−1·g−1) evolution rates of g-C3N4/TiO2are higher than those of g-C3N4and TiO2. The enhanced photocatalytic CO2reduction performance is attributed to the efficient charge carrier transfer in the g-C3N4/TiO2heterojunction. The electron transfer route was verified by in situ irradiated X-ray photoelectron spectroscopy (XPS). The photocatalytic CO2reduction mechanism on g-C3N4/TiO2was investigated by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). This work provides a strategy for designing a polymer/metallic oxide heterojunction with efficient electron transfer for enhanced photocatalytic CO2reduction.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Wenlu Luo,Wei Lu,Qin Xiang,Lianlong Zhan,Xun Yang,Hanbing Jiang,Cailin Xu,Hui He
The utilization of the solar-driven CO 2 desorption of carbon capture materials opens a promising avenue to reduce energy consumption in the carbon capture process. A crucial aspect is the careful coordination of materials' adsorption capacity and regeneration temperature. In this study, a photothermal responsive carbon capture material was developed by incorporating a photothermal responsive cellulose nanofiber matrix skeleton with a temperature-sensitive Pluronic® F-127 and polyethyleneimine. These components formed a staggered network through crosslinking with epichlorohydrin. The devised preparation strategy demonstrated a remarkable conversion rate of 99% for the reaction reagents. The resulting carbon capture material exhibited a high amino density of 14.18 mmol/g and a substantial adsorption capacity of 6.92 mmol/g. Notably, the shrinkage of Pluronic® F-127 molecular chains at elevated temperatures led to an increased surface electrostatic potential and the passivation of amino groups. This transformation endowed the material with a solar-driven regeneration temperature as low as 55 °C, representing an efficient approach to reduce energy consumption during the regeneration process of carbon capture materials.
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CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
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2024
·
IF 5.9
Maomao Liu,Guizeng Liang,Ningce Zhang,Tao Li,Lipeng Diao,Ping Lu,Xiaoliang Zhao,Daohao Li,Dongjiang Yang
Rationally constructed new catalyst can promote carbon dioxide reduction reaction (CO 2 RR) to valuable carbonaceous fuels such as formate and CO, providing a promising strategy for low CO 2 emissions. Herein, the synthesized Ni 3 S 2 @C as a highly efficient electro-catalyst exhibits remarkable selectivity for formate with 73.9% faradaic efficiency (FE) at −0.7 V vs. RHE. At high applied potential, it shows a high syngas evolution with CO/H 2 ratios (0.54–3.15) that are suitable for typical downstream thermochemical reactions . The experimental and theoretical analyses demonstrate that the electron-rich Ni 2+ in Ni 3 S 2 enhances the adsorption behavior of ∗ OCHO intermediate, reduces the energy barrier of the formation of intermediates, and improves the selectivity of the formate product. Attenuated total reflection surface-enhanced infrared absorption spectra conducted in situ show that ∗ OCHO intermediate is more likely to be generated and adsorbed on Ni 3 S 2 , enhancing the selectivity and activity of the formate product.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Ying Wang,Fei Liu,Mengqin Yao,Jun Ma,Shuo Geng,Jianxin Cao,Xiaodan Wang
Promoting the efficient formation of methanol intermediates during CO 2 hydrogenation to lower olefins plays a decisive role in improving the catalytic performance of a tandem catalyst. In this study, a series of chromium (Cr)-modified gallium–zirconium oxides with the formula GaCrZrO x (y%) were prepared via the sol–gel method. The characterization and experimental results show that the addition of moderate amounts of Cr not only facilitates the formation of more oxygen vacancies on the surface of GaZrO x but also strengthens the adsorption and activation ability of CO 2 and H 2 , thereby promoting the generation of formate and methoxy intermediates. After coupling with SAPO-34 zeolite, the methanol intermediate produced on GaCrZrO x (y%) is rapidly converted into lower olefins. This integration manner oxide and zeolite catalysts is particularly important for catalytic performance because an appropriate affinity between components can induce the formation of methanol intermediates via the kinetic effect, which limits the reverse water–gas shift reaction at high temperature. The GaCrZrO x (3.0 %)/SAPO-34 tandem catalyst synthesized via grinding and mixing at 390 °C and 3 MPa exhibits remarkable stability and catalytic performance, achieving a CO 2 conversion close to 30 %, a lower olefin selectivity of 85.8 %, and a lower olefin yield of 11.7 %.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Duoyong Zhang,Chen Zhang,Xinqi Zhang,Yongqiang Tian,Xusheng Cheng,Xuancan Zhu,Liwei Wang
To enhance CO 2 sorption efficiency under low-pressure conditions and effectively compete with N 2 sorption in flue gas, modifications are implemented aimed at improving the adsorption capacity and selectivity of ZIF-8, renowned for their robust stability. Deep eutectic solvent (DES) comprising tetraethylammonium chloride (TEAC), tetrapropylammonium chloride (TPAC), and tetrabutylammonium bromide (TBAB) as hydrogen-bond acceptors, along with ethanolamine (MEA) as the hydrogen-bond donor, were meticulously prepared for this purpose. ZIF-8 underwent modification through DES loading, resulting in the distinctive emergence of a “core-membrane” structure. Characterization revealed that the DES effectively adhered to the surface of ZIF-8 in a membrane-like structure, without altering the chemical structure or pore size of ZIF-8. The most significant enhancement in sorption capacity was observed with TPAC&MEA modification. Considering the presence of N 2 partial pressure in the flue gas, at 0.05 and 1 bar, the CO 2 adsorption capacities reached 1.92 and 3.03 mmol g −1 , respectively, increasing 71.11 and 4.00 times compared to pristine ZIF-8. The ZIF-8 exhibited a CO 2 /N 2 separation coefficient of 72.77, which increased to a maximum of 997.50 after DES modification. Additionally, the modified material demonstrated exceptional cyclic and thermal stability during testing. This study significantly elevates the CO 2 adsorption capacity and selectivity of solid materials within the low-pressure range, providing pivotal support for CO 2 capture and decarbonization efforts.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Dandan Liu,Jinghao Hua,Weijie Zhang,Kai Wei,Shushan Song,Qianyu Wang,Ziheng Song,Huarui Han,Changchang Ma,Sheng Feng
Building efficient catalysts is an urgent issue in the field of photocatalytic CO 2 reduction, and Z-scheme heterojunction structures can availably suppress the recombination of photo generated carriers and improve photocatalytic performance. This study successfully prepared a new type of Bi 4 O 5 Br 2 /Bi-MOF composite photocatalyst through self-assembly method. After 5 h of simulated sunlight exposure, the optimized sample 50-Bi 4 O 5 Br 2 /Bi-MOF photocatalytic reduction of CO 2 to CO efficiency (23.78 μmol·g −1 ·h −1 ) was 5.09 times higher than pure Bi 4 O 5 Br 2 , and the CH 4 yield (5.39 μmol·g −1 ·h −1 ) was 2.52 times that of pure Bi-MOF. In addition, in the cyclic experiment, the catalyst had high stability and reusability. The Z-scheme charge transfer mechanism was confirmed through band structure analysis, Electron spin resonance (ESR), Ultraviolet photoelectron spectroscopy (UPS) and other related characterizations. This work provided an important strategy for designing efficient Z-scheme heterojunction photocatalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Rui Zhai,Zhenyu Wang,Mengyue Gu,Haoliang Liu,Xuewen Zhao,Jiangfan Li,Yaqiong Su,Yonghong Cheng,Shaobin Wang,Jinying Zhang
Selective photoreduction of CO 2 into ethylene is desirable but stays challenging due to easy desorption of primary reduction product CO. Herein, violet phosphorene nanosheets (VPNS) are for the first time demonstrated to be effective CO 2 photoreduction catalysts to yield ethylene. Photoelectron was found to transfer from VPNS to co-catalyst Ag and aggregated on VPNS-Ag interface to enhance CO 2 and CO* adsorption, and further lower the reduction energy barrier to yield ethylene, which was confirmed by in-situ diffuse reflectance infrared Fourier-transform, CO stripping voltammetry, CO reduction experiments, and density functional theory calculations. CO 2 is reduced into COOH* and automatically transformed into CO* on VPNS-Ag surface, then protonized into CHO* with a low barrier of 0.64 eV and automatically coupled into COCHO* to yield ethylene. Only ethylene was detected from CO 2 photoreduction with a yield of 10.34 μmol g −1 h −1 without any hole-sacrificial agent, much higher than most reported photocatalysts.
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Chem
·
2024
·
IF 19.1
Yaolin Wang,Jiaqiang Yang,Yuhai Sun,Daiqi Ye,Bin Shan,Shik Chi Edman Tsang,Xin Tu
Plasma catalysis offers a flexible and decentralized solution for CO 2 hydrogenation to methanol under ambient conditions, avoiding the high temperatures and pressures required for thermal catalysis. However, the reaction mechanism, particularly plasma-assisted surface reactions, remains unclear, limiting the development of efficient catalysts for selective methanol synthesis. Here, we report a bimetallic Ni-Co catalyst effective in plasma-catalytic CO 2 hydrogenation to methanol at 35°C and 0.1 MPa, achieving 46% methanol selectivity and 24% CO 2 conversion. In situ plasma-coupled Fourier transform infrared characterization, along with density functional theory calculations, reveals that the engineered bimetallic sites act as primary active centers for methanol synthesis, promoting the rate-determining step in H-radical-induced reaction pathways by reducing steric hindrance effects. This work demonstrates the significant potential of bimetallic catalysts in plasma-catalytic CO 2 hydrogenation to methanol under ambient conditions, representing a major step toward sustainable CO 2 conversion and fuel production.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Yuying Zhao,Shengchun Hu,Qixin Yuan,Ao Wang,Kang Sun,Ziyun Wang,Mengmeng Fan,Jianchun Jiang
Electrochemical CO 2 conversion into formate by intermittent renewable electricity, presents a captivating prospect for both the storage of renewable electrical energy and the utilization of emitted CO 2 . Typically, Cu-based catalysts in CO 2 reduction reactions favor the production of CO and other by-products. However, we have shifted this selectivity by incorporating B, N co-doped carbon (BNC) in the fabrication of Cu clusters. These Cu clusters are regulated with B, N atoms in a porous carbon matrix (Cu/BN-C), and Zn 2+ ions were added to achieve Cu clusters with the diameter size of ∼1.0 nm. The obtained Cu/BN-C possesses a significantly improved catalytic performance in CO 2 reduction to formate with a Faradaic efficiency (FE) of up to 70 % and partial current density (j formate ) surpassing 20.8 mA cm −2 at −1.0 V vs RHE. The high FE and j formate are maintained over a 12-hour. The overall catalytic performance of Cu/BN-C outperforms those of the other investigated catalysts. Based on the density functional theory (DFT) calculation, the exceptional catalytic behavior is attributed to the synergistic effect between Cu clusters and N, B atoms by modulating the electronic structure and enhancing the charge transfer properties, which promoted a preferential adsorption of HCOO* over COOH*, favoring formate formation.
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ChemSusChem
·
2024
·Vol. 17
·期 16
·e202301951
·
IF 7.5
Kaili Wang,Zhaowei Zhang,Shenyao Wang,Lili Jiang,Haoran Li,Congmin Wang
Graphical CO 2 absorption capacity, desirable absorption enthalpy and excellent reversibility were achieved through dual-tuning azole-based ionic liquids for CO 2 capture from ambient air A strategy of tuning azole-based ionic liquids for reversible CO 2 capture from ambient air was reported. Through tuning the basicity of anion as well as the type of cation, an ideal azole-based ionic liquid with both high CO 2 capacity and excellent stability was synthesized, which exhibited a highest single-component isotherm uptake of 2.17 mmol/g at the atmospheric CO 2 concentration of 0.4 mbar at 30 °C, even in the presence of water. The bound CO 2 can be released by relatively mild heating of the IL-CO 2 at 80 °C, which makes it promising for energy-efficient CO 2 desorption and sorbent regeneration, leading to excellent reversibility. To the best of our knowledge, these azole-based ionic liquids are superior to other adsorbent materials for direct air capture due to their dual-tunable properties and high CO 2 capture efficiency, offering a new prospect for efficient and reversible direct air capture technologies.
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ChemSusChem
·
2024
·
IF 7.5
Chen Liao,Hongwei Zhou,Shunxin Zhang,Feng Wang,Ya Liu,Liejin Guo
Graphical A highly effective photocatalytic system (V Cu −CuInS 2 /MXene) was developed for transforming CO 2 into acetate under full spectrum irradiation. The incorporation of the LSPR effect and defect engineering leads to a highly selective system. Photocatalytic CO 2 conversion towards C 2+ fuels is a promising technology for simultaneously achieving carbon neutrality and alleviating the energy crisis. However, this strategy is inefficient due to the difficulty of both multi-electron transfer and C−C coupling during C 2+ formation. In this work, CuInS 2 /MXene heterostructure with Cu vacancy is rationally designed by in situ hydrothermal synthesis. The V Cu −CuInS 2 /MXene heterostructure has a suitable band structure and tight interface contact. Catalytic performances under different testing conditions, in situ spectroscopy, and COMSOL simulation reveal that LSPR-activated MXene promotes the formation of crucial intermediate CH 2 * and triggers the C−C coupling process under near-infrared light, as the key to acetate. Moreover, in situ XPS analysis, DFT calculations, and photoelectrochemical characterizations unveil that copper vacancy can promote charge transfer from CuInS 2 to MXene and boost local electron aggregation on the MXene, further enhancing the photocatalytic efficiency and selectivity of C 2 products. Contributing to the synergistic effect of copper vacancy and plasmonic MXene, V Cu −CuInS 2 /MXene achieved excellent CO 2 RR activity with an acetate evolution rate of 250.0 μmol/h/g and a selectivity of 97.5 % under the full spectrum irradiation, which is 38.8 and 3.3 times higher than that of V Cu −CuInS 2 and CuInS 2 /MXene, respectively.
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Molecular Catalysis
·
2024
·
IF 3.9
Yingfang Nie,Yu Mei,Youcai Zhu,Yue Mu,Yulong Wu,Li Sun,ZhenHao Xi,Zhen Liu
The copolymerization of carbon dioxide (CO 2 ) and propylene oxide (PO) catalyzed by diethyl zinc/glycerol has been studied by experimental and theoretical approaches. The efficiency of the catalyst is strongly determined by the preparation methods, as the catalyst showed high activity when the catalyst was prepared by dropping glycerol into diethyl zinc. Conversely, the catalyst showed almost no activity when the dropping order was reversed. The order of dropwise addition could change the reaction between diethyl zinc and glycerol, which affects the structure of the catalyst and leads to a change in the catalytic activity. DFT calculations showed that the catalyst is self-assembled and the copolymerization follows a bimetallic coordination-push mechanism.
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