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Greenhouse Gases-Science and Technology · 2022 ·Vol. 12 ·期 3 ·362-375 · IF 2.518

CO2 absorption and microwave regeneration with high-concentration TETA nonaqueous absorbents

Jinxiu Li,Yu Li,Chen Li,Rui Tu,Pengfei Xie,Yi He,Yao Shi

While nonaqueous organic-amine absorbents have great potential in reducing energy consumption of CO 2 capture, their absorption/desorption behaviors are still poorly understood when high-concentration polyamines are used. On the other hand, large scale CO 2 capture demands the use of high-concentration polyamines absorbents. Therefore, we investigated the absorption and microwave regeneration behavior of high-concentration triethylenetetramine (TETA) in three typical organic solvents, including polyethylene glycol 200 (PEG200), diethylene glycol (DEG), and ethylene glycol (EG). The results showed that high-concentration TETA nonaqueous absorbents demonstrate advantages in absorption rate and regeneration energy consumption. The average absorption rate of 2.0 and 5.0 mol/L TETA/EG was 2.84 and 4.70 times that of 0.6 mol/L, respectively. The energy consumption of TETA/EG and TETA/DEG decreased by 29.4 and 25.6% as the concentration increased from 0.6 to 5.0 mol/L. In addition, the high-concentration TETA/PEG200 absorbent demonstrated observable tolerance for water vapor, which usually exists in flue gas. Results also showed that microwave regeneration was superior to conventional conduction heating especially when high-concentration TETA/PEG200 absorbent were used. The energy consumption of microwave regeneration of the absorbent with a concentration of 0.6, 2.0, and 5.0 mol/L was reduced by 65.9, 81.2, and 86.0%, respectively when compared with conduction heating. © 2022 Society of Chemical Industry and John Wiley & Sons, Ltd.

CAS / MDL: 111-46-6 142-58-5
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ACS Omega · 2022 · IF 4.132

CO2-Low Interfacial Tension Viscoelastic Fluid Synergistic Flooding in Tight Reservoirs

Longlong Chen,Xinwei Liao,Shanfa Tang,Shuyun Feng,Ruijia Tang,Shaojing Jiang,Yuanwu Dong

Tight oil reservoirs have poor physical properties, insufficient formation energy, and low natural productivity. CO2 flooding is an important technical mean that enhances the oil recovery of dense reservoirs and achieves effective CO2 sequestration, but strong heterogeneity of the tight oil reservoir usually results in gas channeling and poor enhanced oil recovery effect. The existing methods to prevent gas channeling are mainly to use the small-molecule amine system and the polymer gel system to plug fracture and high permeability channels. The small-molecular amine system has low flash points and pollutes the environment and the polymer gel has poor injectivity and great damage to the formation, which limit their large-scale application. Therefore, a new viewpoint of CO2-low interfacial tension viscoelastic fluid synergistic flooding for enhanced oil recovery in a tight oil reservoir was made. The performance of low interfacial tension viscoelastic fluid (GOBT) was studied. The injectivity and oil displacement effect of CO2-GOBT synergistic flooding were evaluated, and the mechanism of CO2-GOBT synergistic flooding was discussed. The experimental results showed that 0.4% GOBT is a low interfacial tension viscoelastic fluid, which has strong adaptability to the salinity water of tight oil reservoirs (6788–80,000 mg/L), good viscosity stability at different pHs, excellent capacity to emulsify crude oil, and the ability to improve reservoir water wettability. CO2 alternating 0.4% GOBT flooding has good injection ability in cores (Ka = 0.249 mD), and injecting 0.4% GOBT can effectively increase the injection pressure of subsequent CO2 flooding. CO2 alternating 0.4% GOBT flooding can effectively improve water flooding recovery in tight sandstone reservoirs, which is better than CO2 flooding and 0.4% GOBT flooding in both homogeneous and heterogeneous conditions. The mechanisms of CO2 alternating 0.4% GOBT flooding to enhance the oil recovery include that GOBT and CO2 foam block high permeability layers, shunt and sweep low permeability layers, and GOBT emulsify and wash oil. CO2 partially dissolving in GOBT synergistically enhances the core water wettability, which improves GOBT injectability, emulsification, and stripping ability to residual oil.

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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

Sulfurization-derived Cu0–Cu+ sites for electrochemical CO2 reduction to ethanol

Tong Dou,Jiawei Du,Jinqing He,Yiping Wang,Xuhui Zhao,Fazhi Zhang,Xiaodong Lei

The transformation of CO 2 into value-added products is a hot research topic. Metal copper as an electrochemical catalyst shows activity for generating multi-carbon products in CO 2 electroreduction. Herein, Cu 2 S nanorods/copper mesh (Cu 2 S/CM) is successfully fabricated, and exhibits high performance of CO 2 electroreduction to ethanol. At −0.8 V vs RHE , it achieved the Faraday efficiency (FE) of 13.5%, the partial current density of 13.3 mA cm −2 and the yield of 986.4 μmol L −1  h −1 for ethanol. Experiments and theoretical calculations indicated that the high performance is benefits from the high density of Cu 0 and Cu  +  pairs derived from Cu 2 S/CM during CO 2 electroreduction and an appropriate surface Cu 0 /Cu  +  ratio of 0.17. The Cu 0 –Cu + sites facilitate the adsorption of key intermediate *CH 2 CHO and decrease the energy barrier of the ethanol pathway. This work provides not only a new comprehension of CO 2 electroreduction with Cu 2 S catalyst but also a design idea based on Cu 0 –Cu + sites in Cu/Cu 2 S catalyst.

CAS / MDL: 298-14-6
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ACS Sustainable Chemistry & Engineering · 2022 · IF 9.224

Deactivation and Stabilization Mechanism of Photothermal CO2 Hydrogenation over Black TiO2

Yang Li,Zhaojian Zeng,Yuanming Zhang,Yong Chen,Wenjing Wang,Xiaoming Xu,Mengyang Du,Zhaosheng Li,Zhigang Zou

Photothermal catalytic reduction of CO2 is a powerful way to promote carbon neutralization goals. However, there are few reports on the deactivation of the photothermal CO2 reduction reaction. Here, we observed an interesting deactivation phenomenon of photothermal CO2 conversion over TiO2–xHx (black TiO2). Despite the presence of a reducing atmosphere of H2, the oxygen vacancy concentration of TiO2–xHx is reduced, resulting in the deactivation of photothermal CO2 reduction. After Ni is modified onto TiO2–xHx, Ni can activate H2 to form Hs, and the oxygen vacancy concentration of Ni/TiO2–xHx may be maintained, thus solving the deactivation problem in photothermal CO2 hydrogenation.

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EUROPEAN POLYMER JOURNAL · 2022 · IF 5.546

Optimizing CO2 capture and separation in pyrene derived covalent triazine frameworks

Yiming Chen,Xuening Hu,Jun Guo,Zhiyong Guo,Hongbing Zhan,Shaowu Du

Covalent triazine framework (CTF) is widely utilized in lots of porosity related applications such as gas storage, molecule separation and heterogenous catalysis. The permanent porosity and high nitrogen content in the CTF material will greatly promote the affinity between gas molecules and the skeleton. In this work, four covalent triazine framework materials (denoted as Py-CTF-400, Py-CTF-500, TPPy-CTF-400 and TPPy-CTF-500) with high BET surface areas had been successfully constructed by pyrene-based building block under ionothermal reaction conditions using anhydrous ZnCl 2 as the polycyclotrimerization catalyst. The surface area, pore volume/size of CTFs can be simply tuned by varying the synthesis temperature. Among the four CTFs, TPPy-CTF-400 display high specific surface area up to 1753 m 2 /g. The high surface area and nitrogen rich scaffold enable these CTFs to facilitate in CO 2 /N 2 , CO 2 /CH 4 separation. Impressively, the CO 2 /N 2 selectivity of Py-CTF-500 is up to 45.3 (298 K, 1 bar), which is comparable to the highest value calculated by ideal adsorption solution theory (IAST) among CTF based materials. More importantly, as the building units of these CTFs extending from 1,3,6,8-tetracyanopyrene (TPy) to 1,3,6,8-tetrakis(4-cyanophenyl) pyrene (TPPy), their CO 2 /N 2 , CO 2 /CH 4 separation efficiency decreased, which is probably ascribed to the decrescent size of the corresponding pore aperture.

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Journal of Energy Chemistry · 2022 · IF 13.599

Tailoring the interactions of heterostructured Ni4N/Ni3ZnC0.7 for efficient CO2 electroreduction

Junjie Wang,Zhao Li,Zhaozhao Zhu,Jinxia Jiang,Yulan Li,Jinju Chen,Xiaobin Niu,Jun Song Chen,Rui Wu

Electrocatalytic CO 2 reduction into CO has been regarded as one of the most promising strategies for sustainable carbon cycles at ambient conditions, but still faces challenges to achieve both high product selectivity and large current density. Here, we report a Ni 4 N/Ni 3 ZnC 0.7 heterostructured electrocatalyst embedded in accordion-like N-doped carbon through a simple molten salt annealing strategy. The optimal Ni 4 N/Ni 3 ZnC 0.7 electrocatalyst achieves a high CO Faraday efficiency of 92.3% and a large total current density of −15.8 mA cm −2 at −0.8 V versus reversible hydrogen electrode, together with a long-term stability about 30 h. Density functional theory results reveal that the energy barrier for *COOH intermediate formation largely decreased on Ni 4 N/Ni 3 ZnC 0.7 heterostructure compared with Ni 4 N and Ni 3 ZnC 0.7 , thus giving rise to enhanced activity and selectivity. A rechargeable Zn-CO 2 battery is further assembled with Ni 4 N/Ni 3 ZnC 0.7 catalyst as the cathode, which shows a maximum power density of 0.85 mW cm −2 and excellent stability.

CAS / MDL: 108-78-1
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JOURNAL OF CATALYSIS · 2022 · IF 8.047

Regulating iron species compositions by Fe-Al interaction in CO2 hydrogenation

Minjie Xu,Xianglin Liu,Guiyao Song,Yingying Cai,Bianfang Shi,Yitao Liu,Xiaoxu Ding,Zixu Yang,Pengfei Tian,Chenxi Cao,Jing Xu

Different iron species exhibit distinct activity and selectivity in CO 2 hydrogenation reaction. Herein, by controlling calcination temperature, Fe-Al interaction in Na promoted Fe-Al catalysts has been regulated, which further leads to various compositions of iron oxide (FeO x ) and iron carbides (Fe 7 C 3 and Fe 5 C 2 ) after CO activation and CO 2 hydrogenation reaction. The phase compositions and structures of Fe-Al catalysts are carefully distinguished by multiple characterizations, including XRD, XPS, MES and TEM, and the reactivity of different phases is studied with the combination of experiments (kinetics, TP and in situ DRIFTS) and Density Functional Theory (DFT) calculations. Our FeAl350 with the highest FeC x content shows the highest CO 2 conversion of 48.2% and the lowest CO selectivity of 10.1%, and FeAl900 with the highest Fe 5 C 2 / FeC x ratio presents the highest C 5+ selectivity of 44.6%. Finally, a correlation between different compositions of iron species with the activity and selectivity of Fe-based for CO 2 hydrogenation to olefins was established.

CAS / MDL: 7784-27-2 7782-61-8
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ACS Applied Energy Materials · 2022 · IF 6.959

Electrochemical CO2-to-Formate Conversion Over Positive Charge Depleted Tin Sites

Rongcheng Peng,Yang Gao,Hussein A. Younus,Yan Zhang,Wenpeng Ni,Shiguo Zhang

Upgrading CO2 to formate systems is a promising avenue for fuel production, and SnOx is a unique low-cost candidate for this conversion. However, the high oxygen affinity of Sn sites leads to a strong adsorption of O-bound intermediates, resulting in a low efficiency of CO2 reduction. Herein, density functional theory (DFT) calculations confirmed that a H-doping strategy of SnO2 produces partially depleted positive charge Sn sites, weakening the adsorption of HCOO* and boosting the electron transfer kinetics. Experimentally, H-doped commercial SnO2 nanoparticles (H-SnO2) indeed had enhanced intrinsic activity for CO2-to-formate conversion with suppressed hydrogen evolution performance. Remarkably, H-SnO2 achieves over 90.0% formate selectivity within −0.6 to −1.0 V (vs RHE) at the industrial current density of 220 mA cm–2. Electrochemical measurements and in situ Raman spectra analysis together disclosed that H-doping speeds up the kinetic rate for the first electron transfer of CO2 reduction and also promotes formate desorption, resulting in the impressively high current density and selectivity of H-SnO2.

CAS / MDL: 18282-10-5
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Catalysts · 2022 ·Vol. 12 ·期 6 ·672 · IF 4.501

Photocatalytic CO2 Reduction Coupled with Alcohol Oxidation over Porous Carbon Nitride

Chuntian Qiu,Shan Wang,Jiandong Zuo,Bing Zhang

The photocatalytic transformation of CO2to valuable man-made feedstocks is a promising method for balancing the carbon cycle; however, it is often hampered by the consumption of extra hole scavengers. Here, a synergistic redox system using photogenerated electron-hole pairs was constructed by employing a porous carbon nitride with many cyanide groups as a metal-free photocatalyst. Selective CO2reduction to CO using photogenerated electrons was achieved under mild conditions; simultaneously, various alcohols were effectively oxidized to value-added aldehydes using holes. The results showed that thermal calcination process using ammonium sulfate as porogen contributes to the construction of a porous structure. As-obtained cyanide groups can facilitate charge carrier separation and promote moderate CO2adsorption. Electron-donating groups in alcohols could enhance the activity via a faster hydrogen-donating process. This concerted photocatalytic system that synergistically utilizes electron-hole pairs upon light excitation contributes to the construction of cost-effective and multifunctional photocatalytic systems for selective CO2reduction and artificial photosynthesis.Keywords:concerted catalysis;CO2reduction;alcohol oxidation;photocatalysis;metal-free catalyst

CAS / MDL: 420-04-2
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LANGMUIR · 2022 · IF 4.331

Preparation of a Fiber-Like 3D-Structured Adsorbent for CO2 Capture

Yangguan Chen,Guorong Lin,Haorui Liu,Jinrui Zhang,Shuixia Chen

Solid amine adsorbents are promising materials to mitigate global warming. In this study, a commercially available melamine-formaldehyde sponge was adopted as a support to prepare a kind of solid amine adsorbent using polyethylenimine as a functional component and ethylene glycol diglycidyl ether as a cross-linker. The adsorbent, with abundant tunnels and a high amine loading amount, had a high adsorption capacity. When the amine loading was 89.6 wt%, the as-prepared adsorbent showed a high adsorption capacity of 7.29 mmol/g at 20 °C in the presence of water. The spent adsorbent could be easily regenerated by heating it at 90 °C, resulting in lower energy consumption. It has been proved by the Avrami model that physical and chemical adsorption coexist in the adsorption of CO2 on this adsorbent. Simulation with the intraparticle diffusion model has revealed that the rate-controlling step in the adsorption process was the gas film diffusion period when the adsorption temperature was below 30 °C, while it was the adsorption equilibrium period when the adsorption temperature was above 30 °C.

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CANADIAN JOURNAL OF CHEMICAL ENGINEERING · 2022 ·Vol. 101 ·期 5 ·2510-2517 · IF 2.5

A non-cross-linked CO2 foam fracturing fluid with low friction

Wenan Sun,Zhongcong Zhao,Junjie Xiong,Yujian Rong,Jin Bao,Baolei Liu,Zhihao Chen

The hydrophobic associating polymer (MXN-1) was used as a foam stabilizer with optimized supporting additives to solve the problem of high friction in foam fracturing fluid. The basic formula was 0.3% MXN-1 + 0.08% sodium dodecyl sulphate (SDS) + 0.3% B-14 + 1% potassium chloride (KCl) + 0.03% ammonium persulphate (APS). The friction reduction, sand-carrying capacity, gel-breaking performance, and core damage of the fracturing fluid system were studied. The results showed that the proposed system had a unique friction reduction advantage compared with the cross-linked guar gum foam fracturing fluid, and the friction reduction percent reached 62% at a high flow rate. The surface tension of the gel breaking solution was lower than 25 mN/m, and the residue content was about 7 mg/L.

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JOURNAL OF MOLECULAR LIQUIDS · 2022 · IF 6.633

Preparation and thickening mechanism of copolymer fluorinated thickeners in supercritical CO2

Caili Dai,Peng Liu,Mingwei Gao,Zhiyuan Liu,Changlong Liu,Yining Wu,Xiangyu Wang,Shichun Liu,Mingwei Zhao,Hui Yan

Supercritical carbon dioxide (SC-CO 2 ) dry fracturing is considered to be an ideal choice for low permeability, tight and other unconventional reservoir development, because SC-CO 2 has the characteristics of inhibiting water sensitivity damage and improving flowback efficiency. However, the low viscosity of SC-CO 2 limits its application. At present, the most effective way is to thicken CO 2 with thickeners. In this work, seven heptadecafluorodecyl acrylate/styrene (HFDA/STY) copolymers were synthesized, their solubility and thickening properties in SC-CO 2 were evaluated. With the increase of phenyl content in the copolymer, the dissolution pressure and thickening ability of the copolymer in SC-CO 2 increased. The solubility pressure of P(HFDA 0.70 -co-STY 0.30 ) reached 22.2 MPa at 5 wt%, and the viscosity of SC-CO 2 was increased by 297 times. The increase of temperature leads to the increase of molecular thermal motion, which leads to the increase of solubility pressure but the opposite of thickening ability. Molecular dynamics (MD) simulation method was used to reveal the thickening mechanism of SC-CO 2 . The MD simulation results show that fluorocarbon headgroups in copolymers can significantly reduce its dissolution pressure and phenyl group plays the key role in improving the viscosity of CO 2 , which is consistent with laboratory experiment results.

CAS / MDL: 67-56-1
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