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Journal articleHuang Z-Y, Qiu W-J, Wang C-H, et al., 2025,
Reducing optical losses and enhancing charge extraction in Sn-Pb perovskite solar cells with a copolymer hole transport layer
, MATERIALS TODAY ENERGY, Vol: 53, ISSN: 2468-6069 -
Journal articleRoh HJ, Kim JH, Mun WJ, et al., 2025,
Thermoplastic Elastomeric Bottlebrush Copolymer Glue Electrolyte Featuring Dual-Ion Transport Channels and Strong Segregation: Experimental and Simulation Insights
, ADVANCED FUNCTIONAL MATERIALS, ISSN: 1616-301X -
Journal articleItskou I, Sageer SC, Dawson DM, et al., 2025,
Boron-functionalized graphitic carbon nitride materials for photocatalytic applications: effects on chemical, adsorptive, optoelectronic, and photocatalytic properties
, ACS Materials Au, Vol: 5, Pages: 656-674, ISSN: 2694-2461Graphitic carbon nitride (gC3N4, or CN herein) is widely studied as a photocatalyst owing to its ease of synthesis, high stability, and optoelectronic properties. However, its photocatalytic performance often remains limited, and a common approach to tune its function and enhance its performance is by doping. Boron (B) functionalization of CN has showed a potential benefit on photocatalytic performance for several reactions. However, the reason for this improvement and the links between synthesis method, exact B chemical environment, and performance remain unclear. Here, we present a fundamental study that elucidates the influence of (i) B functionalization, (ii) B content, and (iii) choice of B precursor on the physicochemical, adsorptive, optoelectronic, and photocatalytic properties of bulk B-CN. We synthesized two sets of B-CN materials (0.5–11 at% B), using either elemental boron or boric acid as precursors. The samples were characterized using several imaging and spectroscopic techniques, which confirm the integration of B into the material through B–O bonding and the creation of B clusters in the case of the boron precursor, with density functional theory (DFT) calculations supporting our analyses. The distribution of B atoms within B-CN particles remained heterogeneous. Compared to CN, B-functionalized materials show enhanced porosity and CO2 uptake, with similar degrees of light absorption and deeper energy band positions. Transient absorption spectroscopy (TAS) measurements showed that charge carrier populations, lifetimes, and kinetics were not significantly affected by B functionalization; however, at 5 at% B doping, an increase in the concentration of charge carriers was seen. Higher B content enhances the photocatalytic NOx removal under UVA irradiation (almost two-fold) and the selectivity to NO3– from NOx photooxidation, but has no significant effect on CO2 photoreduction, compared to pristine CN. Overall, this study provides fundam
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Journal articleChen L, Qiang T, Daboczi M, et al., 2025,
Ti3C2Tx 2D and 0D MXene Cocatalysts on CuO for Enhanced Photocatalytic Hydrogen Evolution
, Energy and Fuels, Vol: 39, Pages: 11855-11864, ISSN: 0887-0624Cocatalysts play a crucial role in photocatalytic reactions, and titanium carbide MXene (Ti<inf>3</inf>C<inf>2</inf>T<inf>x</inf>) is a promising alternative to expensive noble metal cocatalysts. Herein, we coupled a copper(II) oxide (CuO) semiconductor with Ti<inf>3</inf>C<inf>2</inf>T<inf>x</inf> in two dimensions, nanosheets (T2D) and quantum dots (T0D), forming T2D/CuO and T0D/CuO composite photocatalysts. The effects of size, morphology, and energetics of the different Ti<inf>3</inf>C<inf>2</inf>T<inf>x</inf> forms were investigated in relation to their photocatalytic hydrogen production rates. The T0D/CuO sample achieved a hydrogen production rate of 2174 (±189) μmol g<sup>-1</sup> h<sup>-1</sup>, which is 19 and over 100 times higher than those of T2D/CuO samples and pure CuO, respectively. The enhanced performance of T0D/CuO compared to T2D/CuO can be attributed to a smaller particle size, improved light absorption, larger specific surface area, and a deeper T0D work function promoting charge separation for photocatalytic reactions. These results highlight the impact of the different dimensionalities of titanium carbide MXenes on the photocatalytic performance of composites and point to promising avenues to achieve efficient photocatalytic systems.
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Journal articleChen L, Qiang T, Daboczi M, et al., 2025,
Ti<sub>3</sub>C<sub>2</sub>T<sub> <i>x</i> </sub> 2D and 0D MXene Cocatalysts on CuO for Enhanced Photocatalytic Hydrogen Evolution
, ENERGY & FUELS, Vol: 39, Pages: 11855-11864, ISSN: 0887-0624 -
Journal articleDaboczi M, Eisner F, Luke J, et al., 2025,
Enhanced solar water oxidation and unassisted water splitting using graphite-protected bulk heterojunction organic photoactive layers
, Nature Energy, Vol: 10, Pages: 581-591, ISSN: 2058-7546Polymer donors and non-fullerene acceptors have played an important role as photoactive materials in the development of high-efficiency organic solar cells and have immense potential in devices for direct solar hydrogen generation. However, their use in direct solar water-splitting devices has been limited by their instability in aqueous environment and recombination losses at the interface with catalysts. Here we report anodes containing PM6:D18:L8-BO photoactive layers reaching high solar water oxidation photocurrent density over 25 mA cm−2 at +1.23 V versus reversible hydrogen electrode and days-long operational stability. This was achieved by integrating the organic photoactive layer with a graphite sheet functionalized with earth-abundant NiFeOOH water oxidation catalyst, which provides both water resistance and electrical connection between the catalyst and the photoactive layer without any losses. Using monolithic tandem anodes containing organic PM6:D18:L8-BO and PTQ10:GS-ISO photoactive layers, we achieve a solar-to-hydrogen efficiency of 5%. These results pave the way towards high-efficiency, stable and unassisted solar hydrogen generation by low-cost organic photoactive materials.
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Journal articleDaboczi M, Eslava S, Guijarro N, 2025,
Graphite-protected organic photoactive layer for direct solar hydrogen generation
, NATURE ENERGY, Vol: 10, Pages: 545-546, ISSN: 2058-7546 -
Journal articleCho Y, Yang M, Cui J, et al., 2025,
Analysis of the TiO<sub>2</sub> Photoanode Process Using Intensity Modulated Photocurrent Spectroscopy and Distribution of Relaxation Times
, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, Vol: 147, Pages: 7703-7710, ISSN: 0002-7863- Cite
- Citations: 8
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Journal articleEbri G, Alhashmi E, Baghdadi Y, et al., 2025,
Simultaneous photocatalytic CO2 reduction and C-C coupling of benzyl alcohol under high pressure and supercritical conditions
, CHEMICAL ENGINEERING JOURNAL, Vol: 505, ISSN: 1385-8947- Cite
- Citations: 6
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Journal articleCho Y, He T, Moss B, et al., 2024,
Analyzing the temperature dependence of titania photocatalysis: kinetic competition between water oxidation catalysis and back electron–hole recombination
, ACS Catalysis, Vol: 14, Pages: 16543-16550, ISSN: 2155-5435This study examines the kinetic origins of the temperature dependence of photoelectrochemical water oxidation on nanostructured titania photoanodes. We observe that the photocurrent is enhanced at 50 °C relative to 20 °C, with this enhancement being most pronounced (by up to 70%) at low anodic potentials (<+0.6 V vs RHE). Over this low potential range, the photocurrent magnitude is largely determined by kinetic competition between water oxidation catalysis (WOC) and recombination between surface holes and bulk electrons (back electron–hole recombination, BER). We quantify the BER process by transient photocurrent analyses under pulsed irradiation. Remarkably, we find that the kinetics of BER (∼90 ms half-time) are independent of temperature. In contrast, the kinetics of WOC, determined from the analysis of the photoinduced absorption of accumulated surface holes, are found to accelerate up to 2-fold at 50 °C relative to 20 °C. We conclude that the enhanced photocurrent densities observed in the low-applied potential region result primarily from the accelerated WOC, reducing losses due to the competing BER pathway. At higher applied potentials (>+0.6 V vs RHE), a smaller (∼10%) enhancement in photocurrent density is observed at 50 °C relative to 20 °C. Photoinduced absorption studies, correlated with studies using triethanolamine as a hole scavenger, indicate that this more modest enhancement at anodic potentials primarily results from an enhanced charge separation efficiency. We conclude by discussing the implications of these results for the practical application of photoanodic WOC under solar irradiation, influenced by these temperature-independent and -dependent underlying kinetic processes.
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Journal articleYang M, Oldham L, Daboczi M, et al., 2024,
Advancing hematite photoanodes for photoelectrochemical water splitting: the impact of g-C3N4 supported Ni-CoP on photogenerated hole dynamics
, Advanced Energy Materials, Vol: 14, ISSN: 1614-6832The increasing demand for clean hydrogen necessitates the rapid development of efficient photoanodes to catalyze the water oxidation half-reaction effectively. Here a strategy is introduced to fabricate photoanodes that synergistically combine and leverage the properties of porous Ti-doped hematite (Ti-Fe2O3) and graphitic carbon nitride (g-C3N4) nanosheets anchored with in situ grown Ni-doped CoP co-catalyst (Ni-CoP). The resulting hybrid photoanodes exhibit >7 times higher photocurrent density at +1.23 VRHE compared with Ti-Fe2O3 photoanodes. Comprehensive characterization techniques, including ambient photoemission spectroscopy, intensity-modulated photocurrent spectroscopy, and transient absorption spectroscopy complementarily reveal the key impact of g-C3N4 in these composites with enhanced solar oxygen evolution reaction: The incorporation of g-C3N4 leads to enhanced charge separation through a type-II heterojunction, thereby increasing the hole flux at the surface, and extending the charge carrier lifetime to the ms-s range needed for water oxidation. Additionally, g-C3N4 facilitates efficient transfer of photogenerated holes to the fine Ni-CoP nanoparticles confined in the graphitic matrix for a boosted oxygen evolution reaction. These findings highlight the advantages of complex heterostructure photoanodes and demonstrate a new application of g-C3N4 as a multifunctional support of co-catalysts for future photoanodes with enhanced performance.
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Journal articleBaghdadi Y, Daboczi M, Temerov F, et al., 2024,
A g-C3N4/rGO/Cs3Bi2Br9 mediated Z-schemeheterojunction for enhanced photocatalytic CO2reduction
, Journal of Materials Chemistry A, Vol: 12, Pages: 16383-16395, ISSN: 2050-7488Photocatalytic CO2 reduction plays a crucial role in advancing solar fuels, and enhancing the efficiency of the chosen photocatalysts is essential for sustainable energy production. This study demonstrates advancements in the performance of g-C3N4 as a photocatalyst achieved through surface modifications such as exfoliation to increase surface area and surface oxidation for improved charge separation. We also introduce reduced graphene oxide (rGO) in various ratios to both bulk and exfoliated g-C3N4, which effectively mitigates charge recombination and establishes an optimal ratio for enhanced efficiency. g-C3N4/rGO serves to fabricate a hybrid organic/inorganic heterojunction with Cs3Bi2Br9, resulting in a g-C3N4/rGO/Cs3Bi2Br9 composite. This leads to a remarkable increase in photocatalytic conversion of CO2 and H2O to CO, H2 and CH4 at rates of 54.3 (±2.0) μmole− g−1 h−1, surpassing that of pure Cs3Bi2Br9 (11.2 ± 0.4 μmole− g−1 h−1) and bulk g-C3N4 (5.5 ± 0.5 μmole− g−1 h−1). The experimentally determined energy diagram indicates that rGO acts as a solid redox mediator between g-C3N4 and Cs3Bi2Br9 in a Z-scheme heterojunction configuration, ensuring that the semiconductor (Cs3Bi2Br9) with the shallowest conduction band drives the reduction and the one with the deepest valence band (g-C3N4) drives the oxidation. The successful formation of this high-performance heterojunction underscores the potential of the developed composite as a photocatalyst for CO2 reduction, offering promising prospects for advancing the field of solar fuels and achieving sustainable energy goals.
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Journal articleLewis BF, Huang C, Itskou I, et al., 2024,
Ca-Doped PrFeO<sub>3</sub> Photocathodes with Enhanced Photoelectrochemical Activity
, SOLAR RRL, Vol: 8, ISSN: 2367-198X -
Journal articleTemerov F, Greco R, Celis J, et al., 2024,
Activating 2D MoS2 by loading 2D Cu–S nanoplatelets for improved visible light photocatalytic hydrogen evolution, drug degradation, and CO2 reduction
, Results in Materials, Vol: 22Finding reliable photocatalysts capable of driving reactions using only sunlight is more needed than ever. A variety of strategies to harvest sunlight and convert it into chemical energy have been successfully utilized such as synthesizing nanostructures, using metal nanoparticles, doping, and others. In this work, we discover a facile way to anchor CuS nanoplatelets on 2D MoS<inf>2</inf> by the solvothermal method using ethylene glycol (EG) as both a reduction agent and an exfoliating agent of bulk MoS<inf>2</inf>. Using CuS as a co-catalysis on MoS<inf>2</inf> with their huge surface areas, led to improved photocatalytic activity for three different applications including H<inf>2</inf> evolution, CO<inf>2</inf> reduction, and endosulfan degradation. Specifically, Cu–S@MoS<inf>2</inf> 3% nanocomposite produced 9.86 μmol g<sup>−1</sup> h<sup>−1</sup> of H<inf>2</inf>, 0.48 μmol g<sup>−1</sup> h<sup>−1</sup> of CO and full decomposition of endosulfan within 6 h. The Cu-loaded MoS<inf>2</inf> nanocomposites were thoroughly characterized by spectroscopic (including synchrotron-based spectroscopy) and microscopic methods to understand the formation of Cu–S during the solvothermal process. Moreover, the role of the EG during the synthetic procedure was revealed experimentally and studied theoretically via DFT simulations.
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Journal articleStewart K, Pagano K, Tan E, et al., 2024,
Understanding effects of alkyl side-chain density on polaron formation via electrochemical doping in thiophene polymers
, Advanced Materials, Vol: 36, ISSN: 0935-9648Polarons exist when charges are injected into organic semiconductors due to their strong coupling with the lattice phonons, significantly affecting electronic charge-transport properties. Understanding the formation and (de)localization of polarons is therefore critical for further developing organic semiconductors as a future electronics platform. However, there are very few studies reported in this area. In particular, there is no direct in situ monitoring of polaron formation and identification of its dependence on molecular structure and impact on electrical properties, limiting further advancement in organic electronics. Herein, how a minor modification of side-chain density in thiophene-based conjugated polymers affects the polaron formation via electrochemical doping, changing the polymers’ electrical response to the surrounding dielectric environment for gas sensing, is demonstrated. It is found that the reduction in side-chain density results in a multistep polaron formation, leading to an initial formation of localized polarons in thiophene units without side chains. Reduced side-chain density also allows the formation of a high density of polarons with fewer polymer structural changes. More numerous but more localized polarons generate a stronger analyte response but without the selectivity between polar and non-polar solvents, which is different from the more delocalized polarons that show clear selectivity. The results provide important molecular understanding and design rules for the polaron formation and its impact on electrical properties.
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Journal articleWu D-T, Zhu W-X, Dong Y, et al., 2024,
Enhancing the efficiency and stability of tin-lead perovskite solar cells via sodium hydroxide dedoping of PEDOT:PSS
, small methods, ISSN: 2366-9608Tin-lead (Sn-Pb) perovskite solar cells (PSCs) have gained interest as candidates for the bottom cell of all-perovskite tandem solar cells due to their broad absorption of the solar spectrum. A notable challenge arises from the prevalent use of the hole transport layer, PEDOT:PSS, known for its inherently high doping level. This high doping level can lead to interfacial recombination, imposing a significant limitation on efficiency. Herein, NaOH is used to dedope PEDOT:PSS, with the aim of enhancing the efficiency of Sn-Pb PSCs. Secondary ion mass spectrometer profiles indicate that sodium ions diffuse into the perovskite layer, improving its crystallinity and enlarging its grains. Comprehensive evaluations, including photoluminescence and nanosecond transient absorption spectroscopy, confirm that dedoping significantly reduces interfacial recombination, resulting in an open-circuit voltage as high as 0.90 V. Additionally, dedoping PEDOT:PSS leads to increased shunt resistance and high fill factor up to 0.81. As a result of these improvements, the power conversion efficiency is enhanced from 19.7% to 22.6%. Utilizing NaOH to dedope PEDOT:PSS also transitions its nature from acidic to basic, enhancing stability and exhibiting less than a 7% power conversion efficiency loss after 1176 h of storage in N2 atmosphere.
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Journal articleZhu Z, Daboczi M, Chen M, et al., 2024,
Ultrastable halide perovskite CsPbBr3 photoanodes achieved with electrocatalytic glassy-carbon and boron-doped diamond sheets
, Nature Communications, Vol: 15, ISSN: 2041-1723Halide perovskites exhibit exceptional optoelectronic properties for photoelectrochemical production of solar fuels and chemicals but their instability in aqueous electrolytes hampers their application. Here we present ultrastable perovskite CsPbBr3-based photoanodes achieved with both multifunctional glassy carbon and boron-doped diamond sheets coated with Ni nanopyramids and NiFeOOH. These perovskite photoanodes achieve record operational stability in aqueous electrolytes, preserving 95% of their initial photocurrent density for 168 h of continuous operation with the glassy carbon sheets and 97% for 210 h with the boron-doped diamond sheets, due to the excellent mechanical and chemical stability of glassy carbon, boron-doped diamond, and nickel metal. Moreover, these photoanodes reach a low water-oxidation onset potential close to +0.4 VRHE and photocurrent densities close to 8 mA cm-2 at 1.23 VRHE, owing to the high conductivity of glassy carbon and boron-doped diamond and the catalytic activity of NiFeOOH. The applied catalytic, protective sheets employ only earth-abundant elements and straightforward fabrication methods, engineering a solution for the success of halide perovskites in stable photoelectrochemical cells.
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Journal articleCui J, Daboczi M, Cui Z, et al., 2024,
BiVO<sub>4</sub> Photoanodes Enhanced with Metal Phosphide Co-Catalysts: Relevant Properties to Boost Photoanode Performance
, SMALL, Vol: 20, ISSN: 1613-6810- Cite
- Citations: 19
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Journal articleLiu S-C, Lin H-Y, Hsu S-E, et al., 2024,
Highly reproducible self-assembled monolayer based perovskite solar cells <i>via</i> amphiphilic polyelectrolyte
, JOURNAL OF MATERIALS CHEMISTRY A, Vol: 12, Pages: 2856-2866, ISSN: 2050-7488 -
Journal articleYang M, Cui J, Daboczi M, et al., 2023,
Interplay between Collective and Localized Effects of Point Defects on Photoelectrochemical Performance of TiO<sub>2</sub> Photoanodes for Oxygen Evolution
, ADVANCED MATERIALS INTERFACES, Vol: 10, ISSN: 2196-7350 -
Journal articleFernandez-Catala J, Jussila L, Daboczi M, et al., 2023,
Shape-Controlled Synthesis of Cu<sub>3</sub>TeO<sub>6</sub> Nanoparticles with Photocatalytic Features
, CRYSTAL GROWTH & DESIGN, Vol: 23, Pages: 8828-8837, ISSN: 1528-7483 -
Journal articleDaboczi M, Cui J, Temerov F, et al., 2023,
Scalable All-Inorganic Halide Perovskite Photoanodes with >100 h Operational Stability Containing Earth-Abundant Materials
, ADVANCED MATERIALS, Vol: 35, ISSN: 0935-9648 -
Journal articleBaghdadi Y, Temerov F, Cui J, et al., 2023,
Cs3Bi2Br9/g‑C3N4 direct Z‑scheme heterojunction for enhancedphotocatalytic reduction of CO2 to CO
, Chemistry of Materials, Vol: 35, Pages: 8607-8620, ISSN: 0897-4756Lead-free halide perovskite derivative Cs3Bi2Br9 has recently been found to possess optoelectronic properties suitable for photocatalytic CO2 reduction reactions to CO. However, further work needs to be performed to boost charge separation for improving the overall efficiency of the photocatalyst. This report demonstrates the synthesis of a hybrid inorganic/organic heterojunction between Cs3Bi2Br9 and g-C3N4 at different ratios, achieved by growing Cs3Bi2Br9 crystals on the surface of g-C3N4 using a straightforward antisolvent crystallization method. The synthesized powders showed enhanced gas-phase photocatalytic CO2 reduction in the absence of hole scavengers of 14.22 (±1.24) μmol CO g–1 h–1 with 40 wt % Cs3Bi2Br9 compared with 1.89 (±0.72) and 5.58 (±0.14) μmol CO g–1 h–1 for pure g-C3N4 and Cs3Bi2Br9, respectively. Photoelectrochemical measurements also showed enhanced photocurrent in the 40 wt % Cs3Bi2Br9 composite, demonstrating enhanced charge separation. In addition, stability tests demonstrated structural stability upon the formation of a heterojunction, even after 15 h of illumination. Band structure alignment and selective metal deposition studies indicated the formation of a direct Z-scheme heterojunction between the two semiconductors, which boosted charge separation. These findings support the potential of hybrid organic/inorganic g-C3N4/Cs3Bi2Br9 Z-scheme photocatalyst for enhanced CO2 photocatalytic activity and improved stability.
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Journal articleSena MS, Cui J, Baghdadi Y, et al., 2023,
Lead-free halide perovskite Cs2AgBiBr6/bismuthene composites for improved CH4 production in photocatalytic CO2 reduction
, ACS Applied Energy Materials, Vol: 6, Pages: 10193-10204, ISSN: 2574-0962CO2 photocatalytic conversion into value-added fuels through solar energy is a promising way of storing renewable energy while simultaneously reducing the concentration of CO2 in the atmosphere. Lead-based halide perovskites have recently shown great potential in various applications such as solar cells, optoelectronics, and photocatalysis. Even though they show high performance, the high toxicity of Pb2+ along with poor stability under ambient conditions restrains the application of these materials in photocatalysis. In this respect, we developed an in situ assembly strategy to fabricate the lead-free double perovskite Cs2AgBiBr6 on a 2D bismuthene nanosheet prepared by a ligand-assisted reprecipitation method for a liquid-phase CO2 photocatalytic reduction reaction. The composite improved the production and selectivity of the eight-electron CH4 pathway compared with the two-electron CO pathway, storing more of the light energy harvested by the photocatalyst. The Cs2AgBiBr6/bismuthene composite shows a photocatalytic activity of 1.49(±0.16) μmol g–1 h–1 CH4, 0.67(±0.14) μmol g–1 h–1 CO, and 0.75(±0.20) μmol g–1 h–1 H2, with a CH4 selectivity of 81(±1)% on an electron basis with 1 sun. The improved performance is attributed to the enhanced charge separation and suppressed electron–hole recombination due to good interfacial contact between the perovskite and bismuthene promoted by the synthesis method.
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Journal articleGreco R, Baxauli-Marin L, Temerov F, et al., 2023,
Activation of 2D cobalt hydroxide with 0D cobalt oxide decoration for microplastics degradation and hydrogen evolution
, CHEMICAL ENGINEERING JOURNAL, Vol: 471, ISSN: 1385-8947- Cite
- Citations: 11
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Journal articleMoruzzi F, Zhang W, Purushothaman B, et al., 2023,
Solution-processable polymers of intrinsic microporosity for gas-phase carbon dioxide photoreduction
, Nature Communications, Vol: 14, ISSN: 2041-1723Four solution-processable, linear conjugated polymers of intrinsic porosity are synthesised and tested for gas phase carbon dioxide photoreduction. The polymers’ photoreduction efficiency is investigated as a function of their porosity, optical properties, energy levels and photoluminescence. All polymers successfully form carbon monoxide as the main product, without the addition of metal co-catalysts. The best performing single component polymer yields a rate of 66 μmol h−1 m−2, which we attribute to the polymer exhibiting macroporosity and the longest exciton lifetimes. The addition of copper iodide, as a source of a copper co-catalyst in the polymers shows an increase in rate, with the best performing polymer achieving a rate of 175 μmol h−1 m−2. The polymers are active for over 100 h under operating conditions. This work shows the potential of processable polymers of intrinsic porosity for use in the gas phase photoreduction of carbon dioxide towards solar fuels.
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Journal articleTemerov F, Baghdadi Y, Rattner E, et al., 2022,
A review on halide perovskite-based photocatalysts: key factors and challenges
, ACS Applied Energy Materials, Vol: 5, Pages: 14605-14637, ISSN: 2574-0962A growing number of research articles have been published on the use of halide perovskite materials for photocatalytic reactions. These articles extend these materials’ great success from solar cells to photocatalytic technologies such as hydrogen production, CO2 reduction, dye degradation, and organic synthesis. In the present review article, we first describe the background theory of photocatalysis, followed by a description on the properties of halide perovskites and their development for photocatalysis. We highlight key intrinsic factors influencing their photocatalytic performance, such as stability, electronic band structure, and sorption properties. We also discuss and shed light on key considerations and challenges for their development in photocatalysis, such as those related to reaction conditions, reactor design, presence of degradable organic species, and characterization, especially for CO2 photocatalytic reduction. This review on halide perovskite photocatalysts will provide a better understanding for their rational design and development and contribute to their scientific and technological adoption in the wide field of photocatalytic solar devices.
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Journal articleCui J, Daboczi M, Regue M, et al., 2022,
2D bismuthene as a functional interlayer between BiVO4 and NiFeOOH for enhanced oxygen-evolution photoanodes
, Advanced Functional Materials, Vol: 32, Pages: 1-12, ISSN: 1616-301XBiVO4 has attracted wide attention for oxygen-evolution photoanodes in water-splitting photoelectrochemical devices. However, its performance is hampered by electron-hole recombination at surface states. Herein, partially oxidized two-dimensional (2D) bismuthene is developed as an effective, stable, functional interlayer between BiVO4 and the archetypal NiFeOOH co-catalyst. Comprehensive (photo)electrochemical and surface photovoltage characterizations show that NiFeOOH can effectively increase the lifetime of photogenerated holes by passivating hole trap states of BiVO4; however, it is limited in influencing electron trap states related to oxygen vacancies (VO). Loading bismuthene on BiVO4 photoanodes increases the density of VO that are beneficial for the oxygen evolution reaction via the formation of oxy/hydroxyl-based water oxidation intermediates at the surface. Moreover, bismuthene increases interfacial band bending and fills the VO-related electron traps, leading to more efficient charge extraction. With the synergistic interaction of bismuthene and NiFeOOH on BiVO4, this composite photoanode achieves a 5.8-fold increase in photocurrent compared to bare BiVO4 reaching a stable 3.4 (±0.2) mA cm–2 at a low bias of +0.8 VRHE or 4.7(±0.2) mA cm–2 at +1.23 VRHE. The use of 2D bismuthene as functional interlayer provides a new strategy to enhance the performance of photoanodes.
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Journal articleEslava S, Hintermair U, 2021,
Editorial: Recent advances in water splitting
, CURRENT OPINION IN GREEN AND SUSTAINABLE CHEMISTRY, Vol: 32, ISSN: 2452-2236 -
Journal articleKumar S, Eslava S, 2021,
Mechanochemically synthesized Pb-free halide perovskite-based Cs2AgBiBr6-Cu-RGO nanocomposite for photocatalytic CO2 reduction
, Journal of Materials Chemistry A, Vol: 5/5/21, Pages: 12179-12187, ISSN: 2050-7488Pb-based halide perovskites have recently showed great potential in various applications such as solar cells, optoelectronics and photocatalysis. Despite their high performance, the Pb2+ toxicity along with poor stability hinders long term applications in photocatalysis. Herein, we report mechanochemically prepared Pb-free Cs2AgBiBr6 double perovskite nanoplates and their heterostructure with Cu-loaded reduced graphene oxide (Cu–RGO) for gas-phase photocatalytic CO2 reduction using water vapor as the proton source in the absence of a hole scavenger. The resulting Cs2AgBiBr6–Cu–RGO nanocomposite shows significant photocatalytic activity of 10.7 (±0.6) μmol CH4 g−1 h−1, 1.9 (±0.3) μmol CO g−1 h−1 and 1.0 (±0.2) μmol H2 g−1 h−1, with a CH4 selectivity of 93.0 (±0.5)% on an electron basis with 1 sun and a remarkable apparent quantum efficiency of 0.89 (±0.21)% at 590 nm. A further 32% enhancement in photocatalytic activity on an electron basis is achieved when the light intensity is doubled (2 suns). The high performance was attributed to their improved charge separation and suppressed electron–hole recombination, along with extended visible light absorption, better stability in a humid environment and improved CO2 adsorption. These findings support Cs2AgBiBr6 as a potential Pb-free alternative to conventional halide perovskites for photocatalytic solar-to-fuel conversion and CO2 utilization.
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