ELECTROCHIMICA ACTA
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2022
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IF 7.336
Shuyan Shao,Tao Wen,Ziqun Wang,Xiaoshuang Yin,Ying Liu,Wenzhong Yang,Yun Chen
Electrocatalytic reduction of CO 2 to formate is an extremely attractive route. Here, we developed a SnSe 2 -graphene composite catalyst, and SnSe 2 nanosheets were linked to graphene by Sn-O-C bonds to form complicated hierarchical nanosheet structure. Due to the intrinsic activity of SnSe 2 and the modification of graphene, the catalyst performed excellent electrocatalytic efficacy for the reduction of CO 2 to formate, with a maximum Faraday efficiency up to 95.1% at -0.9 V (vs. RHE) and a current density of 11.8 mA cm −2 under the optimal conditions. Kinetic experiments indicated that the SnSe 2 -graphene composite achieved efficient formate selectivity for CO 2 reduction by increasing the initial transfer rate of electrons to the CO 2 molecule.
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HIGH PERFORMANCE POLYMERS
·
2022
·
IF 1.73
Yihao Nie,Xibin Yi,Xinfu Zhao,Shimo Yu,Jing Zhang,Xiaochan Liu,Sijia Liu,Zhipeng Yuan,Minna Zhang
The cost of CO2 separation and energy consumption can be decreased through the use of CO2 adsorption. Due to the electron-rich heteroatoms in its network, polyimide (PI) has a remarkable affinity for CO2. Polyethylene glycol (PEG) can increase the layer spacing of polymers, so as to change the mass transfer of CO2 in it. Furthermore, the ether bond (-O-) in PEG has good affinity for CO2. In this study, PEG-1000 was introduced into PI aerogel by mild sol-gel method at low temperature, and freeze-drying was used to produce PI/PEG composite aerogels with directional pore structure. The effect of PEG-1000 content and directional pore structure of the PI/PEG composite aerogels on CO2 adsorption performance were further studied. The L-PI/PEG-4 composite aerogel, which contains 4 g PEG and is directionally frozen in liquid nitrogen, has a CO2 adsorption capacity of 16.76 cm3/g at 25°C and 1 bar. L-PI/PEG-4 aerogel also exhibits high CO2/N2 selectivity and adsorption cycle stability.
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APPLIED SURFACE SCIENCE
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2022
·
IF 7.392
Gaosheng Ren,Zhihui Su,Yu Tang,Weichen Du,Nan Xu,Chengyi Dai,Xiaoxun Ma
It is very important to design model catalysts to control the site distribution and develop methods to improve their electronic environment and thus promote the catalyst’s performance in the electrochemical reduction of CO 2 (CO 2 RR). In this work, a strategy of in-situ synthesis and anchoring of nanoparticles (SSAN) was developed. Using this strategy, a “jujube-cake” type catalyst was designed, referred to as Ag@4-MBA. In this catalyst, Ag nanoparticles (NPs) act as “jujube”, which are embedded in 4-mercaptobenzoic acid (4-MBA) acting as “cake”. A Pointer-shaped Ag@4-MBA material was prepared that achieved high loading of Ag species (∼24.0 wt%), high dispersion (5–10 nm), high CO mass activity (93.7 A g Ag −1 ), high CO faradaic efficiency (94.0%) and high CO production (2.0 mol g Ag −1 h −1 ), showing a superior performance to that of the recently reported Ag-based catalysts. Density functional theory (DFT) calculations and X-ray photoelectron spectroscopy (XPS) characterization showed that a high degree of electron delocalization of the Ag–S–aromatic ring and reconstructing the electronic environment of the metal sites were achievied, it is beneficial to stabilize the reaction intermediate COOH*. This work provides a new approach for the design of metal nanoparticle model catalysts with more sustainable CO 2 RR.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Wanfeng Yang,Conghui Si,Yong Zhao,Qingru Wei,Guixing Jia,Guanhua Cheng,Jingyu Qin,Zhonghua Zhang
Antimony (Sb) as a low-toxic and cost-effective metal is a promising material to catalyse CO 2 electroreduction to formate with practical viability. However, monometallic Sb suffers from intrinsically low catalytic activity and the competing hydrogen evolution. Here, we report nanoporous Sb-Bi alloys for substantially improving the catalytic activity of Sb and suppressing hydrogen evolution. The optimal Sb-Bi alloy exhibits a maximum Faradaic efficiency of 95.8 % toward formate production, surpassing the 11.6 % of monometallic Sb counterpart. Operating the catalyst in the flow cell demonstrates a formate partial current density of 734 mA cm −2 and cathodic energy efficiency of 59 % at a moderate overpotential of 800 mV, representing a record formate-production performance so far. Experimental and theoretical studies indicate that the Sb-Bi interactions activate Sb sites to selectively stabilize *OCHO intermediates, facilitating CO 2 -to-formate conversion. This work offers insights in manipulating bimetallic interactions to transform inert materials into active catalysts for efficient electrocatalysis.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2022
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IF 3.898
Ye Yuan,Yurui Pan,Menglong Sheng,Guangyu Xing,Ming Wang,Jixiao Wang,Zhi Wang
Membrane technology features inspiring excellence from numerous separation technologies for CO 2 capture from post-combustion gas. Polyvinylamine (PVAm)-based facilitated transport membranes show significantly high separation performance, which has been proven promising for industrial scale-up. However, commercialized PVAm with low molecular weight and excessive crystallinity is not available to prepare high-performance membranes. Herein, the synthesis process of PVAm was optimized by regulating polymerization and acidic hydrolytic conditions. The membranes based on PVAm with a molecular weight of 154 kDa and crystallinity of 11.37% display high CO 2 permeance of 726 GPU and CO 2 /N 2 selectivity of 55 at a feed gas pressure of 0.50 MPa. Furthermore, we established a PVAm synthesis reactor with an annual PVAm solution (1%(mass)) capacity of over 7000 kg and realized the scaled-up manufacture of both PVAm and composite membranes.
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Journal of CO2 Utilization
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2022
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IF 8.321
Jinsong Shi,Hongmin Cui,Jianguo Xu,Nanfu Yan,Shengyong You
Influences of porous carbon’s physicochemical properties on CO 2 adsorption vary with CO 2 pressure. The clarification of such complicated influences will undoubtedly be beneficial to the design and synthesis of carbonaceous adsorbents. To this end, in the current work we synthesized a series of N-doped hierarchically ordered micro-mesoporous carbons (NHOMCs). Ordered mesoporous polymer was synthesized with a solvent-free method using F127 as the soft template. After removing F127, the polymer was activated with KHCO 3 in the presence of urea at 700–800 °C. The obtained NHOMCs inherited the ordered structure of the polymer, and exhibited high surface area and nitrogen content. Synergistic effects of urea and KHCO 3 on nitrogen content and textural properties were discussed and revealed. At 25 °C, high CO 2 uptakes of 4.02 mmol/g (1 bar) and 15.42 mmol/g (20 bar) were achieved by the NHOMCs. We then systematically investigated the correlation between CO 2 uptake and physicochemical properties. The decisive factors of CO 2 uptakes at different pressures (1 bar, 5 bar, 10 bar, 20 bar) were analyzed. We believe the current work will provide helpful insights into the research of porous carbons for CO 2 adsorption.
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CARBOHYDRATE POLYMERS
·
2022
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IF 10.723
Jinqiang Sun,Mengge Shang,Minna Zhang,Shimo Yu,Zhipeng Yuan,Xibin Yi,Serguei Filatov,Jing Zhang
Biomass aerogels are attractive in various applications owing to their inherent advantages of renewability, biodegradability and eco-friendly. Herein, a novel composite aerogel of konjac glucomannan (KGM)/TEMPO-oxidized cellulose nanofibers (TOCNF)@HKUST-1 (KTA@HKUST-1) is prepared through a facile vacuum impregnation method combined with the directional freeze-drying process, which using KGM and TOCNF as raw materials. The structural analyses disclose that the KTA@HKUST-1 has a hierarchical porosity, in which HKUST-1 can provide micropores for adsorption, while the meso -/macropores from KTA act as high-speed channels to improve diffusion and mass transfer rate to transport CO 2 components into the micropores of HKUST-1. The experiment results of KTA@HKUST-1-10 (KTA@H10) show that the CO 2 adsorption capacity can reach 3.50 mmol·g −1 at 1 bar and 298 K, and the adsorption capacity retention rate as high as 91.43% after 7 cycles. In addition, the CO 2 /N 2 adsorption selectivity of KTA@H10 can reach 18.42, which has an excellent potential for selective CO 2 adsorption.
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PubMed
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-8
·
IF 17.694
Mu Shijia,Lu Honglei,Wu Qianbao,Li Lei,Zhao Ruijuan,Long Chang,Cui Chunhua
Cu δ+ sites on the surface of oxide-derived copper (OD-Cu) are of vital importance in electrochemical CO 2 reduction reaction (CO 2 RR). However, the underlying reason for the dynamically existing Cu δ+ species, although thermodynamically unstable under reductive CO 2 RR conditions, remains uncovered. Here, by using electron paramagnetic resonance, we identify the highly oxidative hydroxyl radicals (OH • ) formed at room temperature in HCO 3 - solutions. In combination with in situ Raman spectroscopy, secondary ion mass spectrometry, and isotope-labelling, we demonstrate a dynamic reduction/reoxidation behavior at the surface of OD-Cu and reveal that the fast oxygen exchange between HCO 3 - and H 2 O provides oxygen sources for the formation of OH • radicals. In addition, their continuous generations can cause spontaneous oxidation of Cu electrodes and produce surface CuO x species. Significantly, this work suggests that there is a “seesaw-effect” between the cathodic reduction and the OH • -induced reoxidation, determining the chemical state and content of Cu δ+ species in CO 2 RR. This insight is supposed to thrust an understanding of the crucial role of electrolytes in CO 2 RR.
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PubMed
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JOURNAL OF MEMBRANE SCIENCE
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2022
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IF 10.53
Huanni Xia,Hua Jin,Yating Zhang,Hao Song,Jianqiao Hu,Yun Huang,Yanshuo Li
Membrane technology with environmentally friendly and cost-efficient features has been well acknowledged as a promising solution for effective CO 2 separation. Metal organic framework (MOF) glasses are one of the most attractive membrane materials currently, because of their easy processability, absence of grain-boundary defects, and permanent porosity. In this study, a mixed linker tetrahedral imidazolate framework-4 (TIF-4) MOF with ultrahigh glass forming ability was selected for fabricating highly CO 2 selective membranes. Through adjusting the molar ratio of the imidazole (Im) and 5-methylbenzimidazolate (5-mbIm) linkers in the TIF-4 framework, the melting temperatures as well as the CO 2 adsorption property could be controlled systematically. After vitrification, TIF-4 glasses (a g TIF-4) with varying 5-mbIm content were prepared, and all of them exhibit higher isosteric heat of CO 2 adsorption than the corresponding TIF-4 crystals. Both CO 2 /CH 4 and CO 2 /N 2 uptake ratio (298 K, 1 bar) of a g TIF-4 samples are more than twice as that of TIF-4 crystals, suggesting the great potential of a g TIF-4 for CO 2 separation. Further, a g TIF-4 membranes were successfully prepared by the melt-quenching process from the polycrystalline membranes. a g TIF-4 membranes are highly CO 2 selective with CO 2 /N 2 and CO 2 /CH 4 separation factors of 27 and 30. More importantly, a g TIF-4 membrane displays long-term stability up to 10 months, which is highly conductive to its industrial application for CO 2 separation.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2022
·Vol. 38
·期 5
·1287-1291
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IF 2.726
Gong Yu,Pan Jing,Zhang Lingling,Wang Xiao,Song Shuyan,Zhang Hongjie
Electrochemical reduction of carbon dioxide into value-added products is a promising way to recycle the greenhouse gas, thus solving the crisis of global warming. Pressing challenges remain in regulating the catalytic selectivity. In this work, we demonstrated a metal-organic frameworks-assisted approach to synthesizing In species loaded on the surface of N doped carbon matrix. By controlling the particle sizes, the catalytic selectivity can be easily altered. The obtained In c /NC possesses the outstanding capability for converting CO 2 into CO. And 80.09% Faraday efficiency (FE) of CO can be achieved at 0.8 V vs. RHE. While the In 2 O 3 /C exhibits different catalytic behaviors, the main product is formic acid and the FE is more than 50% at 0.8 V vs. RHE. The selectivity reversal can be attributed to the strong interactions between In clusters and N atoms of carbon supports, which efficiently inhibits the formation of the by-product, formic acid. Our research has paved a new way to modulate catalytic selectivity by manipulating the fine structures of the catalysts.
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Coatings
·
2022
·Vol. 12
·期 2
·233
·
IF 3.236
Shiyuan Liu,Botao Hu,Junkai Zhao,Wenjun Jiang,Deqiang Feng,Ce Zhang,Wei Yao
The electrocatalytic CO2reduction reaction (CO2RR) into hydrocarbon products is one of the most promising approaches for CO2utilization in modern society. However, the application of CO2RR requires optimizing state-of-the-art catalysts as well as elucidating the catalytic interface formation mechanism. In this study, a flower-like nano-structured Bi catalyst is prepared by a facile pulse current electrodeposition method wherein the morphologies could be accurately controlled. Interestingly, nano-structured Bi is inclined to generate Bi2O2CO3in the air and form a stable Bi2O2CO3@Bi interface, which could enhance the CO2adsorption and conversion. In-situ Raman spectroscopy analysis also proves the existence of Bi2O2CO3on the electrode surface. In a practical CO2reduction test by a flow-cell reactor, the Bi2O2CO3@Bi electrode delivers a high faradaic efficiency of the CO2to formate/formic acid (~90%) at −1.07 V vs. reversible hydrogen electrode (RHE) with no obvious decay during more than a 10 h continuous test. The introducing surface Bi2O2CO3in nano-structured Bi supports a promising strategy as well as facile access to prepare improved CO2RR electrocatalysts.Keywords:CO2reduction;bismuth;Bi2O2CO3;interface;formic acid
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BRAZILIAN JOURNAL OF CHEMICAL ENGINEERING
·
2022
·Vol. 39
·期 3
·661-669
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IF 1.772
Jin Zhengwei,Yu Changjun,Wang Ruyang,Wei Wei,Jing Yunhuan,Wang Qi
The production of precipitated calcium carbonate (PCC) from carbonate-free minerals and CO 2 from industrial exhaust gas could lower energy consumption and promote CO 2 sequestration. The present study proposes a chemical looping process for the production of PCC from wollastonite (calcium silicate) and CO 2 from industrial exhaust using ammonium chloride as the looping medium; this study also included a pilot setup with a capacity of 3 kg of carbonate per hour to demonstrate the process. The process consisted of three phases: extraction of calcium from the wollastonite with hydrochloric acid; carbonation of the CO 2 in the extract solution in the presence of ammonia to produce calcium carbonate while generating ammonium chloride; and regeneration of hydrochloric acid and ammonia by the decomposition of ammonium chloride. A special air-lift reactor with an integrated settling vessel was designed for the carbonation reaction. The extraction and carbonation conditions were optimized, and fine calcium carbonate with a purity greater than 98% and a particle size of 2 μm was produced. The overall utilization of the calcium from wollastonite and the CO 2 reached 99 and 90%, respectively. This process avoids the high-temperature pyrolysis of limestone and thus consumes less energy. It also sequesters CO 2 from industrial exhaust and is a green and high-performing process for the production of PCC.
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