SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Yuhang Yang,Chuanwen Zhao,Pengxin Zeng,Yuhao Wang,Xue Qin,Yueyue Gao,Yafei Guo,Ruilin Wang,Jian Sun
Suitable molding and granulation methods are crucial, and an outstanding sphere structure can play a better role in the future scale-up industrial application of K 2 CO 3 -based CO 2 adsorbent. Water will form a large contact angle on the surface of hydrophobic solution and become sphericity water. In this work, hydrophobic powders (polyethylene (PE), TiO 2 , and SiO 2 ) were selected in the hydrophobic interface-assisted method. The CO 2 adsorption capacity of TiO 2 pellets is 0.50 mmol/g, while that of PE pellets is 0.24 mmol/g, and finally that of SiO 2 pellets is 0.36 mmol/g. Then, experiment proved that high temperature (>500 ℃) makes the hydrophobic powders (i.e, TiO 2 and SiO 2 ) lose hydrophobicity which make water molecules diffuse faster, while PE is completely decomposed at high temperature. Compared with the pellets calcined at 300 ℃, the TiO2 pellets calcinated at 500 ℃ have an adsorption capacity of 0.70 mmol/g, which is over 1.72 times that of the original pellets, and the other two hydrophobic surfaces are also improved to some extent. Additionally, the appropriate ratio of low-temperature pore forming agent (i.e., urea) can help improve the adsorption performance, while excessive addition will lead to poor CO 2 adsorption performance. In addition, the K 2 CO 3 /Al 2 O 3 pellets also exhibited desirable mechanical properties, with an optimal compressive strength of 41 Mpa. Therefore, the loss of hydrophobicity leads to more active diffusion of water molecules, which may provide a new idea for the future development of CO 2 adsorbents and other areas.
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Journal of Energy Chemistry
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2023
·
IF 13.1
Jing Zhang,Jia-Jun Dai,De-Quan Cao,Heng Xu,Xing-Yu Ding,Chun-Hua Zhen,Beate Paulus,Jin-Yu Ye,Qian Liang,Jun-Ke Liu,Shi-Jun Xie,Sai-Sai Deng,Zhen Wang,Jun-Tao Li,Yao Zhou,Shi-Gang Sun
With tunable local electronic environment, high mass density of MN 4 sites, and ease of preparation, metal–organic conjugated coordinative polymer (CCP) with inherent electronic conductivity provides a promising alternative to the well-known M−N−C electrocatalysts. Herein, the coordination reaction between Cu 2+ and 1,2,4,5-tetraaminobenzene (TAB) was conducted on the surface of metallic Cu nanowires, forming a thin layer of CuN 4 -based CCP (Cu-TAB) on the Cu nanowire. More importantly, interfacial transfer of electrons from Cu core to the CuN 4 -based CCP nanoshell was observed within the resulting CuTAB@Cu, which was found to enrich the local electronic density of the CuN 4 sites. As such, the CuTAB@Cu demonstrates much improved affinity to the *COOH intermediate formed from the rate determining step; the energy barrier for C–C coupling, which is critical to convert CO 2 into C 2 products, is also decreased. Accordingly, it delivers a current density of −9.1 mA cm −2 at a potential as high as −0.558 V (vs. RHE) in H-type cell and a Faraday efficiency of 46.4% for ethanol. This work emphasizes the profound role of interfacial interaction in tuning the local electronic structure and activating the CuN 4 -based CCPs for efficient electroreduction of CO 2 .
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RSC Advances
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2023
·Vol. 13
·期 21
·14554-14564
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IF 3.9
Zhong Xie,Jinpei Hei,Chuan Li,Xiaojie Yin,Fengyi Wu,Lei Cheng,Sugang Meng
An activated carbon-supported Cu/ZnO catalyst (CCZ-AE-ox) was successfully obtained by the ammonia evaporation method for the hydrogenation of carbon dioxide to methanol, and the surface properties of the catalyst post-calcination and reduction were investigated. Activated carbon facilitated the increased dispersion of the loaded metals, which promote the CO2 space-time yield (STY) of methanol and turnover frequency (TOF) on the active sites. Furthermore, the factors affecting the catalyst in the hydrogenation of CO2 to methanol were in-depth investigated. The larger surface area and higher CO2 adsorption capacity are found to make possible the main attributions of the superior activity of the CCZ-AE-ox catalyst.
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ACS Sustainable Chemistry & Engineering
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2023
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IF 8.4
Fuying Zhu,Haochen Qiu,Fei Wang,Xing Zhang,Guo-Ping Lu,Yamei Lin,He Huang
CO2 conversion by stable, cost-effective carbonic anhydrase (CA)-like nanozymes emerges as an efficient and sustainable approach for CO2 fixation. In this work, a novel iron-based nanomaterial (Fe10@CN-Mg) was first reported to be a CA mimic, in which FeNx sites and Mg(OH)2 play a synergistically catalytic effect for CO2 conversion. Although this material has much lower metal content and cost, it has comparable kinetic constants (Km 6.37 mM and Vmax 30.74 mM/min) and a significantly higher CaCO3 formation rate (20.60 g·g–1·h–1, the quality of CaCO3 produced per hour per gram of the catalyst) than that of reported CA mimics. Fe10@CN-Mg is stable when processed at extreme pH, high temperature, organic solvents, and high ionic strength and also retains high activity after long storage times (two months) and seven cycles. In addition, Fe10@CN-Mg was successfully applied to convert CO2 into cyclic carbonates with high economic efficiency.
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EcoMat
·
2023
·Vol. 5
·期 5
·e12334
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IF 14.6
Juhee Jang,Shangqian Zhu,Ernest Pahuyo Delmo,Tiehuai Li,Qinglan Zhao,Yinuo Wang,Lili Zhang,Hongwen Huang,Jingjie Ge,Minhua Shao
Despite of superior performance of the oxide-derived copper (OD-Cu) in producing valuable hydrocarbons during CO 2 RR, its fabrication process is still ambiguous and complicated. In this work, we develop a simple microwave-assisted method to synthesize the oxide-derived Cu nanosheet (OD-Cu NS) and reveal that the oxidation state of Cu species is controlled by varying the Cu precursor amount. Notably, the simultaneous formation of nano-sized Cu domains influence the surface roughness of OD-Cu NS. The partially oxidized Cu surface exhibits a superior faradaic efficiency (FE) of C 2+ products up to 72%, along with a partial current density of 55 mA cm −2 in a neutral KHCO 3 solution. More importantly, the as-obtained OD-Cu NS shows a synergetic effect on dissociating of CO 2 molecules by the strong binding energy and promoting of C 2+ compounds productivity by the enlarged electrochemical surface area. This work provides a new insight for designing efficient OD-Cu catalysts toward CO 2 RR.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Tengfei Zhang,Feng He,Jianling Zhang,Fangna Gu
It is challenging to fabricate supported Ni catalysts with more active sites to improve their low-temperature catalytic performance in CO 2 methanation . Herein, firstly, ultrathin (∼4 nm) NiZrAl layered double hydroxide (LDH) nanosheets were synthesized by co-precipitation method, followed by aqueous miscible organic solvent treatment (AMOST), and applied as catalyst precursors for CO 2 methanation. After H 2 reduction, the surface area of Ni particles in NiZrAl-LDH-AMO-R was significantly higher than that of NiZrAl-LDH-R without AMOST. As a result, the NiZrAl-LDH-AMO-R showed higher catalytic activity than NiZrAl-LDH-R owing to its higher H 2 and CO 2 chemisorption capacity and lower activation energy . During the 100 h-lifetime test, NiZrAl-LDH-AMO-R maintained a steady CO 2 conversion of about 92.3%. Moreover, NiZrAl-LDH-AMO-R maintained its catalytic activity after a 600 °C-hydrothermal treatment, suggesting its high stability. In situ DRIFTS results reveal that CO 2 methanation on both NiZrAl-LDH-R and NiZrAl-LDH-AMO-R followed the HCOO∗ route. Interestingly, more active sites obtained after AMOST strongly promoted the generation and decomposition of HCOO∗, and thus significantly improved the activity of NiZrAl-LDH-AMO-R at low temperatures.
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CATALYSIS LETTERS
·
2022
·Vol. 153
·期 11
·3383-3391
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IF 2.936
Zhang Luping,Tu Xuewei,Han Weihang,Chen Liangchen,Chen Yutong,Zheng Hui
As the main resource of greenhouse gas, CO 2 needs to be fixed into different chemicals to relieve the environmental problem. Fe-based catalyst and g-C 3 N 4 have received extensive attention due to their easy preparation, low cost, and environmental friendliness. Herein, a heterogeneous catalyst system consisting of rich-electron g-C 3 N 4 and strong electron-withdrawing groups Fe-complex [Fe(bpy)(CO) 2 (Cl) 2 ] was developed, which could promote electron transfer and enhance the electronic interaction for fixing CO 2 . o -phenylenediamine substrates with different electron-donating/withdrawing groups were employed to fix CO 2 into high-valued heterocycle benzimidazoles. The optimum reaction conditions were examined by orthogonal experiments. A series of benzimidazole derivatives were synthesized with yield up to 98%, which indicated the catalyst had the ability of fixing CO 2 . This catalyst provides a new pathway for fixing CO 2 into valuable benzimidazole derivatives. Graphical Abstract
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CHINESE JOURNAL OF CATALYSIS
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2022
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IF 12.92
Yuehui Li,Duanhui Si,Wangyin Wang,Song Xue,Wenzhe Shang,Zhanyou Chi,Can Li,Ce Hao,Govindjee Govindjee,Yantao Shi
For natural oxygenic photosynthesis, there is a consensus that H 2 O is oxidized to molecular oxygen by photosystem II (PSII) in the grana, while CO 2 assimilation takes place, long after oxygen evolution, in light-independent reactions, for example, through the Calvin-Benson Cycle in the stroma. Here, we report, for the first time, light-driven CO 2 assimilation by the PSII core complex, where the formation of methanol, along with the oxygen evolution, is validated by in - situ mass spectrometry, gas chromatography and isotopic labeling experiments. Such an unusual CO 2 assimilation is likely to be a simultaneous event along with the usual electron transfer occurring in normal light–independent assimilation. This discovery is extraordinary and is of great significance as it may substantially modify our understanding of the mechanism of photosynthesis.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Zhizhou Cai,Ning Cao,Fanxing Zhang,Xiangzhou Lv,Ke Wang,Yi He,Yao Shi,Hao Bin Wu,Pengfei Xie
Electrocatalytic CO 2 reduction into ethanol driven by renewable energy represents a promising strategy for energy storage and mitigation of global warming, but it has remained challenging to gain high activity and selectivity of ethanol. Here we take advantage of atomic arrangement in immiscible Ag-Cu composite during annealing and establish hierarchical interfaces in the obtained core-shell catalyst. The atomic Ag-Cu interactions increase electrochemical surface area and expedite charge dynamics, resulting in an unprecedented electrocatalytic performance with the faradaic efficiency of C 2+ products, ethanol as 80.2 %, 52.6 % and the current density of ∼320 mA cm −2 at −1.0 V (versus reversible hydrogen electrode). Moreover, the Ag-Cu catalyst exhibits a notable stability for ∼60 h. Mechanism studies reveal that local CO intermediates preferentially accumulate on the core, then migrate to the continuous Cu surface for C-C coupling energy-favorably toward ethanol. Our work highlights a novel design principle as interface engineering for advanced tandem electrocatalysts.
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Membranes
·
2023
·Vol. 13
·期 2
·166
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IF 4.2
Jingfeng Li,Zeyu Cao,Bo Zhang,Xinai Zhang,Jinchao Li,Yaping Zhang,Hao Duan
CO is a significant product of electrochemical CO2reduction (ECR) which can be mixed with H2to synthesize numerous hydrocarbons. Membranes, as separators, can significantly influence the performance of ECR. Herein, a series of quaternized polybenzimidazole (QAPBI) anion exchange membranes with different quaternization degrees are prepared for application in ECR. Among all QAPBI membranes, the QAPBI-2 membrane exhibits optimized physico-chemical properties. In addition, the QAPBI-2 membrane shows higher a Faraday efficiency and CO partial current density compared with commercial Nafion 117 and FAA-3-PK-130 membranes, at −1.5 V (vs. RHE) in an H-type cell. Additionally, the QAPBI-2 membrane also has a higher Faraday efficiency and CO partial current density compared with Nafion 117 and FAA-3-PK-130 membranes, at −3.0 V in a membrane electrode assembly reactor. It is worth noting that the QAPBI-2 membrane also has excellent ECR stability, over 320 h in an H-type cell. This work illustrates a promising pathway to obtaining cost-effective membranes through a molecular structure regulation strategy for ECR application.
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ChemCatChem
·
2023
·Vol. 15
·期 4
·e202201413
·
IF 4.5
Dandan Zhao,Shaoyang Zhang,Tianyu Guo,Qiang Zhao,Jianping Du,Jinping Li
Graphical Carbon dioxide reduction : The rectangular nanoflakes with crystalline/amorphous phase structures that the square nanoblocks are confined in amorphous nanoflakes efficiently enhance the electrocatalytic conversion of CO 2 to ethylene. The electrocatalytic reduction of CO 2 to high value-added chemicals is one of the effective technologies to achieve the goal of carbon neutralization. However, highly selective production of hydrocarbon via electrochemical conversion of CO 2 still has great challenges. Herein, a unique CuO phase composition is constructed that consists of rectangular nanoflakes possessing crystalline/amorphous structures by the facile strategy. Crystalline CuO square nanoblocks are confined in amorphous nanoflakes and form crystalline/amorphous hybrid phase. The results of electrocatalytic CO 2 reduction demonstrate that this crystalline/amorphous CuO material exhibits superior CO 2 conversion ability with ethylene Faradaic efficiency of 58.3 % at −1.08 V vs. RHE, which is ascribed to nanoflake structures and fast electron transfer on the crystalline/amorphous interfaces because of superior conductivity of amorphous CuO. The present research provides an effective route to reconstruct novel crystalline/amorphous interfaces of CuO for catalysis applications.
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JOURNAL OF MEMBRANE SCIENCE
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2022
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IF 10.53
Nan Li,Zhi Wang,Jixiao Wang
Carbonic anhydrase (CA)-inspired membranes for CO 2 separation were constructed by introducing hydroxypropyl-β-cyclodextrins (Hβ-CDs) into the polyamide networks, which were formed via interfacial polymerization reactions between trimesoyl chloride and tertiary amino-containing monomers . Hydrophobic inner cavities of Hβ-CDs with the hydrophilic exterior can be used to simulate the hydrophobic pockets of CA enzymes. Hydrophilic and hydrophobic regions were constructed via introducing Hβ-CDs into membranes, while the transport of nonpolar CO 2 molecules and polar components (H 2 O and HCO 3 − ) in CO 2 hydration reactions could be enhanced. Meanwhile, tertiary amino groups in biomimetic membranes can act as the base catalysts for CO 2 hydration reactions, which were deemed as carriers for facilitated transport membranes. Biomimetic membranes containing Hβ-CDs and tertiary amino groups exhibited outstanding CO 2 permeance of 2792 GPU and CO 2 /N 2 selectivity of 171 at 0.15 MPa, showing the potentials for low-pressure CO 2 capture. Particularly, CO 2 transport mechanisms were also analyzed for biomimetic facilitated-transport membranes, which can supply new visions for developing novel membrane materials for CO 2 separation.
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