Probing dissolved CO2(aq) in aqueous solutions for CO2 electro-reduction and storage

2022 ◽  
Author(s):  
Jiachen Li ◽  
Jinyu Guo ◽  
Hongjie Dai
Keyword(s):  
Aqueous Solutions ◽  
Co2 Capture ◽  
High Pressures ◽  
Dynamic Monitoring ◽  
State Transitions ◽  
Ir Absorption ◽  
Large Hysteresis ◽  
Co2 Electroreduction ◽  
First Time

CO2 dissolved in aqueous solutions is of wide ranging importance from CO2 capture, storage and photo-/electro-reduction in the fight against global warming, to CO2 analysis in various liquids including natural waterbodies and consumer drinking products. Here we developed micro-scale infrared (IR) spectroscopy for in-situ dynamic monitoring and quantitating CO2(aq) in aqueous solutions with high time resolutions under various conditions including CO2 gas bubbling and high pressures. The quantized CO2(g) rotational state transitions were observed to quench when dissolved in water to form CO2(aq) solvated by water molecules, accompanied by increased H2O IR absorption. An accurate CO2 molar extinction coefficient ε was derived for in-situ CO2(aq) quantification up to 58 atm. For the first time, we directly measured CO2(aq) concentrations in electrolytes under CO2(g) bubbling and high pressure conditions. In KHCO3 electrolytes with CO2(aq) > ~ 1 M, CO2 electroreduction (CO2RR) to formate reaches > 98% Faradaic efficiencies on copper (Cu2O/Cu) based electrocatalyst. Further, we probed CO2 dissolution/desolvation kinetics important to energy and environmental applications dynamically, revealing large hysteresis and ultra-slow reversal of CO2(aq) supersaturation in water, with implications to CO2 capture, storage and supersaturation phenomena in natural water bodies.

scholarly journals Direct CO2 Electroreduction from Carbonate

2019 ◽  
Author(s):  
Yuguang Li ◽  
Geonhui Lee ◽  
Tiange Yuan ◽  
Ying Wang ◽  
DaeHyun Nam ◽  
...  
Keyword(s):  
Co2 Capture ◽  
Carbon Utilization ◽  
System A ◽  
Carbonate Formation ◽  
Co2 Electroreduction ◽  
Cell Energy ◽  
Co2 Valorization ◽  
Ag Catalyst ◽  
Conversion Technologies

The process of CO2 valorization – all the way from capture/concentration of CO2 to its electrochemical upgrade - requires significant inputs in each of the capture, upgrade, and separation steps. The gas-phase CO2 feed following the capture-and-release stage and into the CO2 electroreduction stage produce a large waste of CO2 (between 80 and 95% of CO2 is wasted due to carbonate formation or electrolyte crossover) that adds cost and energy consumption to the CO2 management aspect of the system. Here we report an electrolyzer that instead directly upgrades carbonate electrolyte from CO2 capture solution to syngas, achieving 100% carbon utilization across the system. A bipolar membrane is used to produce proton in situ, under applied potential, which facilitates CO2 releasing at the membrane:catalyst interface from the carbonate solution. Using an Ag catalyst, we generate pure syngas at a 3:1 H2:CO ratio, with no CO2 dilution at the gas outlet, at a current density of 150 mA/cm2, and achieve a full cell energy efficiency of 35%. The direct carbonate cell was stable under a continuous 145 h of catalytic operation at ca. 180 mA/cm2. The work demonstrates that coupling CO2 electrolysis directly with a CO2 capture system can accelerate the path towards viable CO2 conversion technologies.

Synthesis of sodium polyacrylate–bentonite using in situ polymerization for Pb2+ removal from aqueous solutions

RSC Advances ◽  
2016 ◽  
Vol 6 (53) ◽  
pp. 48145-48154 ◽  
Author(s):  
Youjun He ◽  
Meishan Pei ◽  
Ni Xue ◽  
Luyan Wang ◽  
Wenjuan Guo
Keyword(s):  
Heavy Metal ◽  
Aqueous Solutions ◽  
Metal Ions ◽  
Heavy Metal Ions ◽  
In Situ Polymerization ◽  
Sodium Polyacrylate ◽  
First Time

A sodium polyacrylate–bentonite material (PAANa–Bent), as an adsorbent for heavy metal ions, is synthesized for the first time using in situ polymerization.

scholarly journals New insight on the simultaneous H2 and HNO2 production in concentrated HNO3 aqueous solutions under alpha radiation

RSC Advances ◽  
2021 ◽  
Vol 11 (20) ◽  
pp. 12141-12152
Author(s):  
Raluca M. Musat ◽  
Jean-Luc Roujou ◽  
Vincent Dauvois ◽  
Muriel Ferry ◽  
Carole Marchand ◽  
...  
Keyword(s):  
Aqueous Solutions ◽  
Precise Determination ◽  
Alpha Radiation ◽  
System P ◽  
Set Up ◽  
First Time

For the first time ever, a specially designed set-up, coupled to the CEMHTI cyclotron allowed in situ monitoring of HNO2 and precise determination of H2 production in the external α radiolysis of HNO3 solution, while ensuring no perturbation of the investigated system.

Anion effects in the formation of the active catalyst in the Ruhrchemie – Rhône-Poulenc aqueous biphasic hydroformylation process. Are there any?

2005 ◽  
Vol 83 (6-7) ◽  
pp. 1033-1036 ◽  
Author(s):  
József Kovács ◽  
Ferenc Joó ◽  
Carl D Frohning
Keyword(s):  
Aqueous Solutions ◽  
Active Catalyst ◽  
Water Soluble ◽  
Catalyst Precursor ◽  
Solution Ph ◽  
Aqueous Biphasic ◽  
First Time ◽  
Close Analogue

The water soluble [Rh(OAc)(CO)(mtppms)2] containing monosulfonated triphenylphosphine ligands was prepared for the first time and its hydrogenation was studied in aqueous solutions. In the presence of additional mtppms, the reaction yielded [RhH(CO)(mtppms)3], a close analogue of [RhH(CO)(mtppts)3], the immediate catalyst precursor in the Ruhrchemie – Rhône-Poulenc aqueous biphasic hydroformylation process. The extent of the [Rh(OAc)(CO)(mtppms)2] → [RhH(CO)(mtppms)3] transformation strongly depended on the solution pH, similar to the case of the hydrogenation of [RhCl(CO)(mtppms)2] studied earlier. In this respect, RhCl3·aq and Rh(OAc)3·aq can be used equally well for the in situ preformation of [RhH(CO)(mtppts)3], although the latter is the preferred choice in the industrial process.Key words: rhodium, water-soluble, hydrides, sulfonated phosphines, biphasic.

scholarly journals Direct CO2 Electroreduction from Carbonate

2019 ◽  
Author(s):  
Yuguang Li ◽  
Geonhui Lee ◽  
Tiange Yuan ◽  
Ying Wang ◽  
DaeHyun Nam ◽  
...  
Keyword(s):  
Co2 Capture ◽  
Carbon Utilization ◽  
System A ◽  
Carbonate Formation ◽  
Co2 Electroreduction ◽  
Cell Energy ◽  
Co2 Valorization ◽  
Ag Catalyst ◽  
Conversion Technologies

The process of CO2 valorization – all the way from capture/concentration of CO2 to its electrochemical upgrade - requires significant inputs in each of the capture, upgrade, and separation steps. The gas-phase CO2 feed following the capture-and-release stage and into the CO2 electroreduction stage produce a large waste of CO2 (between 80 and 95% of CO2 is wasted due to carbonate formation or electrolyte crossover) that adds cost and energy consumption to the CO2 management aspect of the system. Here we report an electrolyzer that instead directly upgrades carbonate electrolyte from CO2 capture solution to syngas, achieving 100% carbon utilization across the system. A bipolar membrane is used to produce proton in situ, under applied potential, which facilitates CO2 releasing at the membrane:catalyst interface from the carbonate solution. Using an Ag catalyst, we generate pure syngas at a 3:1 H2:CO ratio, with no CO2 dilution at the gas outlet, at a current density of 150 mA/cm2, and achieve a full cell energy efficiency of 35%. The direct carbonate cell was stable under a continuous 145 h of catalytic operation at ca. 180 mA/cm2. The work demonstrates that coupling CO2 electrolysis directly with a CO2 capture system can accelerate the path towards viable CO2 conversion technologies.

scholarly journals Determination of Cadmium (II) in Aqueous Solutions by In Situ MID-FTIR-PLS Analysis Using a Polymer Inclusion Membrane-Based Sensor: First Considerations

Molecules ◽  
2020 ◽  
Vol 25 (15) ◽  
pp. 3436 ◽  
Author(s):  
René González-Albarrán ◽  
Josefina de Gyves ◽  
Eduardo Rodríguez de San Miguel
Keyword(s):  
Aqueous Solutions ◽  
Analytical Sensitivity ◽  
Concentration Difference ◽  
Inclusion Membrane ◽  
Polymer Inclusion Membrane ◽  
Pls Analysis ◽  
First Time

Environmental monitoring is one of the most dynamically developing branches of chemical analysis. In this area, the use of multidimensional techniques and methods is encouraged to allow reliable determinations of metal ions with portable equipment for in-field applications. In this regard, this study presents, for the first time, the capabilities of a polymer inclusion membrane (PIM) sensor to perform cadmium (II) determination in aqueous solutions by in situ visible (VIS) and Mid- Fourier transform infrared spectroscopy (MID-FTIR) analyses of the polymeric films, using a partial least squares (PLS) chemometric approach. The influence of pH and metal content on cadmium (II) extraction, the characterization of its extraction in terms of the adsorption isotherm, enrichment factor and extraction equilibrium were studied. The PLS chemometric algorithm was applied to the spectral data to establish the relationship between cadmium (II) content in the membrane and the absorption spectra. Furthermore, the developed MID-FTIR method was validated through the determination of the figures of merit (accuracy, linearity, sensitivity, analytical sensitivity, minimum discernible concentration difference, mean selectivity, and limits of detection and quantitation). Results showed reliable calibration curves denoting systems’ potentiality. Comparable results were obtained in the analysis of real samples (tap, bottle, and pier water) between the new MID-FTIR-PLS PIM based-sensor and F-AAS.

Probing the Dynamic Self-Assembly Behaviour of Photoswitchable Wormlike Micelles in Real Time

2018 ◽  
Author(s):  
Elaine A. Kelly ◽  
Judith E. Houston ◽  
Rachel Evans
Keyword(s):  
Real Time ◽  
Absorption Spectroscopy ◽  
Self Assembly ◽  
Uv Light ◽  
Wormlike Micelles ◽  
Tetraethylene Glycol ◽  
Light Illumination ◽  
First Time ◽  
Dependent Processes

Understanding the dynamic self-assembly behaviour of azobenzene photosurfactants (AzoPS) is crucial to advance their use in controlled release applications such as<i></i>drug delivery and micellar catalysis. Currently, their behaviour in the equilibrium <i>cis-</i>and <i>trans</i>-photostationary states is more widely understood than during the photoisomerisation process itself. Here, we investigate the time-dependent self-assembly of the different photoisomers of a model neutral AzoPS, <a>tetraethylene glycol mono(4′,4-octyloxy,octyl-azobenzene) </a>(C<sub>8</sub>AzoOC<sub>8</sub>E<sub>4</sub>) using small-angle neutron scattering (SANS). We show that the incorporation of <i>in-situ</i>UV-Vis absorption spectroscopy with SANS allows the scattering profile, and hence micelle shape, to be correlated with the extent of photoisomerisation in real-time. It was observed that C<sub>8</sub>AzoOC<sub>8</sub>E<sub>4</sub>could switch between wormlike micelles (<i>trans</i>native state) and fractal aggregates (under UV light), with changes in the self-assembled structure arising concurrently with changes in the absorption spectrum. Wormlike micelles could be recovered within 60 seconds of blue light illumination. To the best of our knowledge, this is the first time the degree of AzoPS photoisomerisation has been tracked <i>in</i><i>-situ</i>through combined UV-Vis absorption spectroscopy-SANS measurements. This technique could be widely used to gain mechanistic and kinetic insights into light-dependent processes that are reliant on self-assembly.

The Total Synthesis of Rhabdastrellic Acid A

2018 ◽  
Author(s):  
Yaroslav Boyko ◽  
Christopher Huck ◽  
David Sarlah
Keyword(s):  
Total Synthesis ◽  
Late Stage ◽  
Cross Coupling ◽  
Side Chains ◽  
General Strategy ◽  
Modular Approach ◽  
Linear Sequence ◽  
Generating Sequence ◽  
First Time

<div>The first total synthesis of rhabdastrellic acid A, a highly cytotoxic isomalabaricane triterpenoid, has been accomplished in a linear sequence of 14 steps from commercial geranylacetone. The prominently strained <i>trans-syn-trans</i>-perhydrobenz[<i>e</i>]indene core characteristic of the isomalabaricanes is efficiently accessed in a selective manner for the first time through a rapid, complexity-generating sequence incorporating a reductive radical polyene cyclization, an unprecedented oxidative Rautenstrauch cycloisomerization, and umpolung 𝛼-substitution of a <i>p</i>-toluenesulfonylhydrazone with in situ reductive transposition. A late-stage cross-coupling in concert with a modular approach to polyunsaturated side chains renders this a general strategy for the synthesis of numerous family members of these synthetically challenging and hitherto inaccessible marine triterpenoids.</div>

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