Ian Sullivan's research while affiliated with California Institute of Technology and other places
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Publications (16)
A comparative study on the solar-to-fuel (STF) conversion efficiency of electrochemical and thermochemical approaches for methane (CH 4), methanol (MeOH), and ethanol (EtOH) generation using sunlight and air was performed. The system level STF conversion efficiency studied herein took into account of both the conversion processes and feedstock capt...
Photoelectrochemical (PEC) water-splitting systems have the unique ability to produce renewable hydrogen directly from sunlight, independent of the electrical grid. These systems are therefore appealing technological options for resilient long-term energy storage. Ion selective membranes, such as monopolar and bipolar membranes, are a vital compone...
Carbon capture from both stationary emitters and dilute sources is critically needed to mitigate climate change. Carbon dioxide separation methods driven by electrochemical stimuli show promise to sidestep the high energy penalty and fossil-fuel dependency associated with conventional pressure and temperature swings. Compared to a batch process, el...
In the version of this article, there were errors in Fig. 2a and d. In Fig. 2a, we have changed Cu2+ to Cu(0) in the revised version. While the two references cited in our paper used Cu2+ in their schematics,1,2 we believe that Cu(0) is the correct representation for the electrochemically mediated amine regeneration (EMAR)3. To be clear, the Cu met...
Electrochemical CO2 conversion into fuels or chemicals and CO2 capture from point or dilute sources are two important processes to address the gigaton challenges in reducing greenhouse gas emissions. Both CO2 capture and electrochemical CO2 conversion are energy intensive, and synergistic coupling between the two processes can improve the energy ef...
Three-dimensional (3D) printed, hierarchically porous nickel molybdenum (NiMo) electrocatalysts were synthesized and evaluated in a flow-through configuration for the hydrogen evolution reaction (HER) in 1.0 M KOH(aq) in a simple electrochemical H-cell. 3D NiMo electrodes possess hierarchically porous structures because of the resol-based aerogel p...
Capture and conversion of CO 2 from anthropogenic emission is becoming an increasingly important social responsibility as the concentration of atmospheric CO 2 continues to rise above record high levels. To achieve carbon negative conditions in the long term, capture and extraction of CO 2 directly from air and seawater will likely play a much bigg...
The rational design of high-performance electrocatalysts requires a detailed understanding of dynamic changes in catalyst properties, including oxidation states, surface area, and morphology under realistic working conditions. Oxide-derived Cu catalysts exhibit a remarkable selectivity towards multi-carbon products for the electrochemical CO reduct...
Capture and conversion of CO2 from oceanwater can lead to net-negative emissions and can provide carbon source for synthetic fuels and chemical feedstocks at the gigaton per year scale. Here, we report a direct coupled, proof-of-concept electrochemical system that uses a bipolar membrane electrodialysis (BPMED) cell and a vapor-fed CO2 reduction (C...
The rational design of high-performance electrocatalysts requires a detailed understanding of dynamic changes in catalyst properties, including oxidation states, surface area, and morphology under realistic working conditions. Oxide-derived Cu catalysts exhibit a remarkable selectivity towards multi-carbon products for the electrochemical CO reduct...
Solar-driven reduction of carbon dioxide represents a carbon neutral pathway for the synthesis of fuels and chemicals. We report here results for solar-driven CO2 reduction using a gas diffusion electrode (GDE) directly powered by a photovoltaic cell. A GaInP/GaInAs/Ge triple junction photovoltaic cell was used to power a reverse-assembled gas diff...
A hybrid catalyst-bonded membrane device using gaseous reactants for carbon monoxide reduction (COR) reaction in the cathode chamber, an aqueous electrolyte for oxygen evolution reaction (OER) in the anode chamber, and an anion exchange membrane (AEM) for product separation was constructed. The Cu electrocatalyst was electrodeposited onto the gas d...
A solar-driven V^(3+/2+)(aq,H_2SO_4)|KOH(aq) cell, consisting of a carbon-cloth cathode in 2.0 M H_2SO_4(aq) with 0.36 M V_2(SO_4)_3 (pH = -0.16), a Ni mesh anode in 2.5 M KOH(aq) (pH = 14.21) for the oxygen-evolution reaction (OER), and a bipolar membrane that sustained the pH differentials between the catholyte and anolyte, enabled water splittin...
A solar-driven V3+/2+(aq,H2SO4)|KOH(aq) cell, consisting of a carbon-cloth cathode in 2.0 M H2SO4(aq) with 0.36 M V2(SO4)3 (pH = -0.16), a Ni mesh anode in 2.5 M KOH(aq) (pH = 14.21) for the oxygen-evolution reaction (OER), and a bipolar membrane that sustained the pH differentials between the catholyte and anolyte, enabled water splitting with spa...
Citations
... However, the incumbent wet chemical scrubbing methods for carbon dioxide (CO 2 ) separation are technically and economically challenged by various inherent limitations, including high energy consumption for sorbent regeneration, thermal degradation, complexity in heat integration when retrofitting existing infrastructures, process equipment corrosion, and fugitive emission of volatile toxic sorbents to the environment 4,5 . Alternatively, electrochemically mediated carbon capture (EMCC) has emerged as a promising technology [6][7][8][9][10][11] . In EMCC, reversible CO 2 capture and release is modulated by switching electrochemical potentials. ...
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... 3,[23][24][25] The polarization curve of a FB-BPM mediating acid-base recombination is shown in Figure 1b. These polarization curves are traditionally collected using 4-probe electrochemical cells with linear sweep voltammetry or galvanostatic measurements, 26 and are typically characterized by a sharp increase in current starting from the open-circuit potential (OCP) until a voltageindependent plateau in current density is reached (ilim). 17 The performance of FB-BPMs can be characterized by these two values (OCP and ilim). ...
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... Gold is a commonly used material for the working electrode and the contact angle for planar gold with water is 45°. 34,35 The bres of biomass skins have a natural ability to resist water. The contact angle for sugarcane skin with water is ∼78°and the contact angle of water droplets on the WE of SugarcaneSens is ∼80° (Fig. S6 †). ...
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... If these limitations are addressed, this technology could become a key method for extracting next-generation Li. It is crucial to develop processes that convert CO 2 to achieve carbon neutrality [59]. The production of Li2CO3 can be derived from three primary sources: hard rock mining, brine extraction, and recycling. ...
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... [3][4][5] As an important factor to the climate change, the CO 2 emissions must decline in the near future and, subsequently, the CO 2 concentration in the atmosphere should as well decrease. [1,3,[6][7][8] Considering the new ambitious targets of the UAE Consensus and the current sustainability policies, only the decrease in emissions will not be enough to reach the established goals. Therefore, the capture of CO 2 is an alternative approach to deplete the concentration of CO 2 in the atmosphere. ...
... [136] Recently, confocal microscopy with photoacids has emerged as a viable technique for measuring the pOH (-log 10 [OH À ], equivalent to pH for OH À ions) within porous gas diffusion layers. [137,138] With Ag electrodes an increase in thickness of the porous electrode from 0.5 to 2.7 μm increased the FE from 5 to 80 % at À 0.7 V vs RHE (Figure 3c). This was postulated, and later shown by multiphysics modelling to be due to the local pH within the electrode acting to suppress H 2 evolution within the porous structure (Figure 3d). ...
... [31][32][33] Through the utilization of available data, various geometric structures can be designed, and 3D printing technology can be used for the fabrication of electrode electrocatalysts, leading to the economical and efficient development of all-in-one electrodes. [34,35] One of the widely used 3D printing technologies, digital light processing (DLP), is characterized by its high precision, low cost, and remarkable efficiency. [36][37][38] Leveraging this technology, macroscopically ordered hole electrode scaffolds can be precisely 3D printed layer by layer. ...
... Because the catalyst's chemical state and the local environment are sensitive to the reaction rate, the nature of the catalyst must be monitored under high practical current densities. For example, a recent report conducted in a gas-fed device revealed no correlation between Cu oxidation state and catalyst performance, ruling out the role of Cu 2 O or CuO in the enhanced activity and selectivity toward C 2 H 4 (44). This critical finding emphasizes the importance of operando analysis at high reaction rates, where the role of the oxidized species in CO 2 RR performance remains unclear. ...
... An alternative, more efficient, and innovative approach involves the direct extraction of CO 2 from the ocean utilizing a bipolar membrane electrodialysis unit and a vapor-fed CO 2 reduction cell. This method yields both an acidified solution and a basified solution, which can subsequently be combined to achieve a neutral-pH solution [141][142][143]. Lithium hydroxide can also be used for CO 2 removal from submarine atmosphere, with good adsorption rates, however, the lithium carbonate formed could not be regenerated [144]. ...
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... A small percentage of Cu 1+ , besides Cu 0 , on the catalyst in the MEA seems to generate an electrostatic tension between the two surface sites that promote the C-C coupling mechanism, favouring the dimerisation pathway for producing C 2 H 4 . This result agrees with previous research findings by Drisdell et al. [34] who assessed the selectivity towards multicarbon products of oxide-derived Cu catalysts tested in a MEA configuration. Operando X-ray absorption spectroscopy (XAS) measurements demonstrated that the C 2 H 4 selectivity increased as Cu 0 increased on the catalyst surface. ...
