ACS Omega
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2023
·
IF 4.1
Xintong Wang,Jiang Yang,Xu Chen,Kunfeng Yan
Two food flavors, furfuryl mercaptan (2-FFT) and difurfuryl disulfide (DFDS), were investigated as green corrosion inhibitors for the N80 steel in a CO2-saturated solution containing 3.5% NaCl. Experimental methods, quantum chemical calculations, and molecular dynamics simulation were employed to evaluate the effectiveness of 2-FFT and DFDS. The results of the study indicate that both 2-FFT and DFDS act as mixed corrosion inhibitors, with a dominant inhibition effect on the cathodic reaction. 2-FFT is physiochemically adsorbed on the steel surface in a tiled form through the furan ring and the – SH groups as adsorption sites. On the other hand, DFDS is chemisorbed on the steel surface through the – S–S– groups in a parallel manner. DFDS exhibits a higher tendency for electron transfer and stronger adsorption to steel compared to 2-FFT. Overall, this study highlights the potential of natural food flavors as effective and environmentally friendly corrosion inhibitors for carbon steel in CO2-saturated environments. The findings of this research can contribute to the development of sustainable and nontoxic corrosion inhibitors for the oil and gas industry.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
·
IF 5.2
Lipei Fu,Ziran Zhang,Xinxin Qiu,Yufei Zheng,Minglu Shao,Yingrui Bai,Zhangkun Ren,Wenzhe Si,Jiafeng Jin,Yanyu Xu,Kaili Liao
A novel rapidly switchable CO 2 /N 2 -responsive Pickering emulsifier based on supramolecular amphiphilic surfactants (SDOA) and nano-SiO 2 has been fabricated. SDOA was constructed by mixing Jeffamine D-230 and oleic acid (HOA) at 1:1 stoichiometric ratio. Compared with conventional small-molecule emulsifiers, the novel rapidly switchable CO 2 /N 2 -responsive Pickering emulsifier was prepared with inexpensive raw materials by a simple method, and there was no contaminant generation during synthesis. A new CO 2 /N 2 -responsive Pickering emulsion was prepared on this basis, and its stable performance and responsiveness were investigated in depth. The results show that this emulsion can be stable for a long time (more than 30 days) at a low surfactant dosage (0.5 mmol/L) through in situ hydrophobization of SiO 2 nanoparticles by hydrogen bonding and electrostatic adsorption. In addition, the emulsion broke rapidly and completely after 10 s of CO 2 introduction into the stable emulsion, and the emulsion could be reconstructed in response to N 2 purging for 5 min at 60 ℃ followed by homogenization . The switching behavior of the emulsion is due to decomposition of the pseudo amphiphile by bubbling CO 2 into the system and both the protonated D-230 ions and the neutral HOA produced have no in situ hydrophobization to SiO 2 particles. At 60 ℃, the influx of N 2 will drive out CO 2 , making HOA re-transform into hydroxide ion, and after re-combining with D-230 ion, it can again perform in-situ hydrophobization on SiO 2 particles, thus forming a stable emulsion. Thanks to the ability of SiO 2 nanoparticles and D-230 ions to maintain electrostatic adsorption after the passage of CO 2 , compared with previous studies, the emulsion can be completely demulsified at a higher pH value (about 5.5), fewer bicarcarbonate roots are formed, less CO 2 needs to be introduced, and N 2 required to re-stabilize the emulsion is also reduced. This greatly increases the response efficiency of the emulsion and reduces the energy loss and the cost of putting the emulsion system into practical application. This research has important implications for fossil fuel generation, production and transportation of crude oil, and other areas.
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CARBON
·
2023
·
IF 10.9
Qiuchan Li,Lang He,Yubin Zeng,Yan Zhao,Mingyue Ding
Obtaining highly active and selective target products is both promising and challenging, and can be achieved by regulating the adsorption and desorption energy of reaction intermediates, as well as the transfer of electrons under visible light. Herein, an efficient CNGA/CdS photocatalyst based on ultrathin porous nitrogen vacancies carbon nitride (CNGA) nanosheets (thickness <1 nm) with CdS nanoparticles was synthesized by a facile route for visible-light photocatalytic CO 2 reduction. As a result, the rate of CO production was 32.75 μmol g −1 h −1 , which was 17.24 and 32.75 times that of CN and CdS under visible light (λ ≥ 420 nm) without sacrificial agents and cocatalysts . Importantly, introducing CdS nanoparticles into CNGA could improve the selectivity of CO 2 to CO by nearly 100% (yield-based selectivity). Finally, the photocatalytic mechanism was explored by in-situ FTIR spectra and DFT calculations, and the results presented that the formation of heterostructures facilitated the generated *CO groups to modulate the reaction pathway of photocatalytic CO 2 reduction. This work is expected provide a reference for the design of photocatalysts for photoreduction CO 2 with accurate products under visible light.
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FUEL
·
2023
·
IF 7.4
Shanshan Shao,Yifan Wang,Laixin Ma,Ziheng Huang,Xiaohua Li
The improved CO 2 adsorption capacity and selectivity is the focus of research on the carbon-based CO 2 adsorbent, while nitrogen-containing groups on the surface of adsorbent have an important effect on the CO 2 adsorption. In this study, nitrogen self-doped hierarchical porous carbon was prepared from three kinds of crustacean shells, namely, hairy crab shell, crayfish shell and greasyback shrimp shell. It revealed that the pore structure of porous carbon can be regulated well with the varied activation temperature and the amount of KOH. With the favorable activation temperature of 800℃ and the mass ratio of activator to carbon (A/C) of 1:1, the obtained porous carbon with different carbon precursors exhibited relatively high specific surface area (1430.63–1734.64 m 2 /g), large pore volume (0.70–1.48 cm 3 /g) and developed pore-size distribution. Consequently, among the three kinds of hierarchical porous carbon tested, that prepared form greasyback shrimp displayed the excellent CO 2 adsorption of 5.144 and 4.325 mmol/g at 1 bar, 273 K and 298 K and the highest CO 2 /N 2 selectivity was observed of 32.32, attributed to the volume of mesopore and micropore and the type of nitrogen-containing groups. The effects of nitrogen-containing groups in porous carbon on the CO 2 adsorption and CO 2 /N 2 selectivity were analyzed, and it revealed that the CO 2 /N 2 selectivity of porous carbon was positively correlated with pyrrolic N. In conclusion, the porous structures and nitrogen-containing groups of porous carbons both contribute to the CO 2 adsorption and selectivity. The porous carbon with well recycling performance in this study presented a practical application prospect.
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Small
·
2023
·Vol. 19
·期 49
·2304084
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IF 13.3
Xiaolei Wang,Wenqian Wang,Bowen Liu,Zichen Song,Zhiyu Ren,Honggang Fu
Although the electron-withdrawing effect of gold (Au) is highlighted in catalytic reactions, its enhancement mechanism for electron transport, especially in the electrochemical process, is still unclear. Herein, Au-decorated Bi 2 O 3 (Au-Bi 2 O 3 ) is proposed as a proof-of-concept to investigate the electron-withdrawing effect in the electrocatalytic CO 2 reduction reaction (eCO 2 RR) process. Evidence from in situ Raman spectra and in situ XRD tests reveals that, compared to Bi 2 O 3 , Bi species in Au-Bi 2 O 3 can be reduced to metallic Bi more rapidly and more easily driven by the electron-withdrawing effect of Au. The XPS tests after eCO 2 RR further validates the transformation from Bi 3+ to Bi 0 in Au-Bi 2 O 3 is more complete. Meanwhile, in the in situ Fourier transform infrared (FTIR) spectra, the key intermediates (CO 2 * − and OCHO* − ) appear at the more positive potential, indicating that metallic Bi is favorable for eCO 2 RR due to the lower energy barrier as corroborated by density function theory (DFT) calculations. Au don't directly participate in the conversion from CO 2 to formate as the reaction sites, but utilize the electron-withdrawing effect to motivate Bi-sites to deliver higher catalytic activity and higher selectivity to formate at a lower applied potential. This study not only has an insight into the electron-withdrawing effect of Au on the eCO 2 RR process, but also develops a new perspective for engineering electron-withdrawing effect in electrocatalysts for high-efficient CO 2 -to-formate conversion.
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INORGANIC CHEMISTRY
·
2023
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IF 4.6
Encheng Liu,Zhenzhen Wang,Zhonghua Sun,Zhihui Zhang,Mingyang He,Qun Chen,Junfeng Qian
The chemical microenvironment modulation of active sites holds promise for facilitating their catalytic performance. Herein, single-atom Ru anchored by ZrSBA-15 modified with diverse organic amine groups has been fabricated and enabled CO2 hydrogenation to produce formic acid (FA) under mild conditions. However, the reaction cannot be achieved without the modification of organic amines. The functional groups as the microenvironment around Ru active sites effectively regulated the activity, in which Ru encapsulated in ZrSBA-15 bearing –NH2 groups exhibited the highest activity, with turnover number (TON) and turnover frequency (TOF) values of 505 and 64 h–1, respectively. Both characterization and experimental results validated that the functional group manipulated the adsorption capacity of the reactant, the electronic state of Ru and hydrophilicity/hydrophobicity of the materials, and thus the catalytic performance.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ke Wang,Jie Chen,Tianyu Wang,Jie Hong,Pengfei Zhao,Edward J. Anthony
Capture and conversion of CO 2 from optimal-scenarios into fuels or chemicals provide a viable solution to combat climate change in reducing greenhouse gas emissions. Here, we propose and experimentally demonstrate that synergistic integration (Catalytic calcium-looping (CaL) gasification of biochar) can realize the capture and in situ conversion of CO 2 . Thermodynamic and kinetic estimations, catalytic conversion and cyclic tests and microstructure characterizations showed that by using a mixture of limestone and K 2 CO 3 -impregnated biochar, calcination fully coupled with the reverse Boudouard reaction can shift thermodynamic equilibrium and simultaneously induce the synergetic catalysis between CaCO 3 and K 2 CO 3 , allowing for accelerating decarbonation kinetics, enhancing CO yield and maintaining stable cyclic CO 2 conversion at lower temperatures (850 °C), as compared to the individual CaL and gasification processes. Theoretical calculations further revealed that the activation energy barriers for the monatomic C-assisted CO 2 dissociation were lower than its desorption energy for CO 2 on the K-doped CaO surface, demonstrating superior conversion reactivity. Importantly, the process is demonstrated in terms of practical scalability using a renewable and cost-effective reductant (biochar), a cheap catalyst (K 2 CO 3 ) and inexpensive natural CO 2 sorbents (limestone and dolomite) in an energy-efficient manner, therefore opening a unique direction for net-negative emission for large CO 2 stationary sources eliminating the need for sequestration.
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Small
·
2023
·Vol. 19
·期 45
·2302022
·
IF 13.3
Hai-Bing Zhao,Jia-Nan Huang,Qi Qin,Hong-Yan Chen,Dai-Bin Kuang
Rational design and facile synthesis of efficient environmentally friendly all-inorganic lead-free halide perovskite catalysts are of great significance in photocatalytic CO 2 reduction. Aiming at photogenerated charge carrier separation and CO 2 reaction dynamics, in this paper, a CsCuCl 3 /Cu nanocrystals (NCs) heterojunction catalyst is designed and synthesized via a simple acid-etching solution process by using Cu 2 O as the sacrificed template. Due to the disproportionation reaction of Cu 2 O induced by concentrated hydrochloric acid, Cu NCs can be deposited onto the surface of CsCuCl 3 microcrystals directly and tightly. As revealed by photoelectrochemical analysis, in situ Fourier transform infrared spectra, etc., the Cu NCs contribute a lot to extracting photoelectrons of CsCuCl 3 to improve the charge separation efficiency, regulating the CO 2 adsorption and activation, and also stabilizing the reaction intermediates. Therefore, CsCuCl 3 /Cu heterojunction exhibits a total electron consumption rate of 58.77 µmol g −1 h −1 , which is 2.9-fold of that of single CsCuCl 3 . Moreover, high CH 4 selectivity of up to 92.7% is achieved, which is much higher than that of CsCuCl 3 (50.4%) and most lead-free halide perovskite-based catalysts. This work provides an ingenious but simple strategy to rationally design cocatalysts in situ decorated perovskite catalysts for manipulating both the catalytic activity and the product selectivity.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Yuying Zhao,Qixin Yuan,Kang Sun,Ao Wang,Ruting Xu,Jing Xu,Yan Wang,Mengmeng Fan,Jianchun Jiang
Carbon material is considered a promising electrocatalyst for the CO2 reduction reaction (CO2RR); especially, N-doped carbon material shows high CO Faradic efficiency (FECO) when using pyridinic N species as the active site. However, in the past decade, more efforts were focused on the preparation of various carbon nanostructures containing abundant pyridinic N species and few researchers studied the electronic structure modulation of the pyridinic N site. The curvature of the carbon substrate is an easily controllable parameter for modulating the local electronic environment of catalytic sites. In this research, carbon nanotubes (CNTs) with different diameters are applied to modulate the electronic environment of pyridinic N by the curvature effect. The pyridinic N sites doped on CNTs with the average curvature of 0.04 show almost 100% FECO at the current density of 3 mA cm–2 at −0.6 V vs RHE and 91% FECO retention after 12 h test, which is superior to most of the carbon-based electrocatalysts. As demonstrated by density functional theory simulation, the pyridinic N site forms a strong local electric field around the nearby C active site and protrudes out of the curved CNT surface like a tip, which remarkably enriches the protons around the adsorbed CO2 molecule.
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Small
·
2023
·Vol. 19
·期 45
·2303405
·
IF 13.3
Mengping Liu,Ganbing Zhang,Ruiqi Ming,Xin Fu,Ruiyi Jiang,Lihong Tian,Xiaobo Chen
Defects on metal oxide have attracted extensive attention in photo-/electrocatalytic CO 2 reduction. Herein, porous MgO nanosheets with abundant oxygen vacancies (V o s) and three-coordinated oxygen atoms (O 3c ) at corners are reported, which reconstruct into defective MgCO 3 ·3H 2 O exposing rich surface unsaturated -OH groups and vacancies to initiate photocatalytic CO 2 reduction to CO and CH 4 . In consecutive 7-cycle tests (each run for 6 h) in pure water, CO 2 conversion keeps stable. The total production of CH 4 and CO attains ≈367 µmol g cata −1 h −1 . The selectivity of CH 4 gradually increases from ≈3.1% (1 st run) to ≈24.5% (4 th run) and then remains unchanged under UV-light irradiation. With triethanolamine (3.3 vol.%) as the sacrificial agent, the total production of CO and CH 4 production rapidly increases to ≈28 000 µmol g cata −1 in 2 h reaction. Photoluminescence spectra reveal that V o s induces the formation of donor bands to promote charge carrier seperation. A series of trace spectra and theoretical analysis indicate Mg-V o sites in the derived MgCO 3 ·3H 2 O are active centers, which play a crucial role in modulating CO 2 adsorption and triggering photoreduction reactions. These intriguing results on defective alkaline earth oxides as potential photocatalysts in CO 2 conversion may spur some exciting and novel findings in this field.
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CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Xuan Li,Xingxing Jiang,Yan Kong,Jianju Sun,Qi Hu,Xiaoyan Chai,Hengpan Yang,Chuanxin He
Electrocatalytic CO 2 reduction reaction (eCO 2 RR) to obtain formate is a promising method to consume CO 2 and alleviate the energy crisis. Indium-based electrocatalysts have demonstrated considerable potential to produce formate. However, their unsatisfactory long-term stability and selectivity restrict their widespread application. In this study, a heterostructure of GaN- and In 2 O 3 -encapsulated porous carbon nanofibers was constructed via electrospinning and the phase transition of eutectic gallium-indium during calcination . The GaN and In 2 O 3 nanoparticle-encapsulated porous carbon nanofibers, when used as electrocatalysts for eCO 2 RR, displayed high formate selectivity with a faradaic efficiency of 87% and maximum partial current density of 29.7 mA cm −2 in a 0.5 mol L −1 KHCO 3 aqueous solution. The existence of the interface can cause a positive shift in the In 3 d binding energy, leading to electronic redistribution. Moreover, the GaN component induced a higher proportion of O-vacancy sites in the In 2 O 3 phase, resulting in improved selectivity for CO 2 -to-formate. In-situ Raman experiments and density functional theory calculations revealed that the interface between GaN and In 2 O 3 could lower the adsorption energy of the key intermediates for formate production, thus providing superior eCO 2 RR performance. In addition, the framework of the porous carbon nanofibers exhibited a large electrochemically active surface area, which enabled the full exposure of the active sites. This study highlights the cooperation between GaN and In 2 O 3 components and provides new insights into the rational design of catalysts with high CO 2 -to-formate conversion efficiencies.
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LANGMUIR
·
2023
·
IF 3.9
Zhen Zhao,Lu Zhang,Hao Zhang,Guoqiang Lu,Tong Meng,Hongguo Hao,Yongmin Zhang,Jun Li,Hui Yan
The superamphiphiles exhibit broad prospects for fabricating stimuli-responsive emulsions. Because the superamphiphiles are assembled via noncovalent interactions, they have the advantage of fast response and high efficiency. Recently, a series of switchable emulsions using CO2-responsive superamphiphiles have been developed, which extends the applications of CO2-responsive materials in widespread field. However, there is still a lack of fundamental understanding on the switching mechanism related to the assembled structure of superamphiphiles at the oil–water interface. We employed molecular dynamics (MD) simulations to investigate the reversible emulsification/demulsification process of a responsive emulsion system stabilized by a recently developed responsive superamphiphile (BTOA), which consists of oleic acid (OA) and cationic amine (named 1,3-bis(aminopropyl)tetramethyldisiloxane, BT). The simulation results present the morphologies in both the emulsion and demulsification states. It is found that the ionized OA– and the protonated BT+ together form an adsorption layer at the oil–water interface. The hydrophobic parts of BT+ are inserted into the adsorption layer, and the two amine groups contact the water phase. This adsorption layer reduces the interfacial tension and stabilizes the emulsion. After the bubbling of CO2, the surfactants were fully protonated to OA and BT2+. Because of the changes in the molecular polarity, OA and BT2+ entered the oil and water phases, respectively, resulting in demulsification. The structural and dynamical properties were analyzed to reveal the different intermolecular interactions that were responsible for the reversible reversibility of the emulsion. The observations are considered to be complementary to experimental studies and are expected to provide deeper insights into studies on developing responsive materials via supramolecular assemblies.
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