Sustainable Energy & Fuels最新文献

{"title":"Nanocomposite electrodes with CuFe layered double hydroxides and hydrochar for alkaline HER and HOR: a multifunctional platform for hydrogen electrocatalysis","authors":"Michelle Saliba, Philippe Knauth, Emily Bloch, Luca Pasquini, Emanuela Sgreccia, Riccardo Narducci, Alessandra Varone and Maria Luisa Di Vona","doi":"10.1039/D6SE00103C","DOIUrl":"https://doi.org/10.1039/D6SE00103C","url":null,"abstract":"<p >The hydrogen evolution reaction (HER) and hydrogen oxidation reaction (HOR) in alkaline media remain limited by slow kinetics and the reliance on noble metal catalysts. Copper-iron layered double hydroxides (CuFe-LDHs), composed of non-rare and low-toxicity elements, offer a sustainable alternative, though their performance is restricted by low conductivity and limited accessibility of active sites. In this work, CuFe-LDHs were synthesized hydrothermally and modified through three complementary strategies: ammonium fluoride (NH<small>₄</small>F) as a structure-directing agent poly(2,6-dimethyl-1,4-phenylene oxide) functionalized with trimethylammonium (PPO-LC) as a hydroxide-conducting ionomer, and a nitrogen-doped hydrochar derived from pine needles as an electron-conducting additive. Structural tuning with 1.5% NH<small>₄</small>F produced highly crystalline LDH-1.5 with increased exposure of catalytic centers, while PPO-LC enhanced OH<small>⁻</small> transport and electrode integrity. Hydrochar contributed additional conductive domains, facilitating charge transfer and improving electrode architecture. The materials were characterized using BET surface area analysis, scanning electron microscopy with EDS element mapping, X-ray diffraction, and Fourier-transform infrared spectroscopy. All catalytic electrodes demonstrated a high electrochemically active surface area. The LDH-1.5/PPO-LC electrode delivered the best HER activity with an overpotential of −332 mV at −10 mA cm<small>⁻²</small>. For the HOR, hydrochar-containing electrodes displayed reduced onset potential values: the LDH-1.5/PPO-LC/HC composite reached the lowest onset potential of 38 mV, though the current densities remained limited. Tafel analysis indicated that the HER is governed by the Volmer step associated with water dissociation, whereas the HOR follows a Heyrovsky–Volmer or Tafel–Volmer pathway depending on the electrode composition. These results highlight the effectiveness of combining structural, ionic, and electronic modifications to enhance the performance of CuFe-LDH-based bifunctional electrodes in alkaline environments, while indicating that further optimization is required to overcome intrinsic kinetic limitations.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 9","pages":" 2314-2326"},"PeriodicalIF":4.1,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/se/d6se00103c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147826924","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A cobalt phthalocyanine-Ketjen black hybrid electrocatalyst for efficient and stable alkaline water splitting","authors":"Shantharaja Daniel and Hyun Chul Kim","doi":"10.1039/D6SE00207B","DOIUrl":"https://doi.org/10.1039/D6SE00207B","url":null,"abstract":"<p >This study aims to develop a sustainable energy framework focused on the evolution of energy conversion and storage applications with excellent performance using lower-cost materials. Some of the electrochemical methods include water electrolysis (the hydrogen evolution reaction [HER] and oxygen evolution reaction [OER]), fuel cells, and metal–air batteries, which are eco-friendly in terms of production of hydrogen and electricity from sustainable sources, and are not only catalytically efficient but also have higher durability. Therefore, the purpose of this research is to develop novel metal-based molecular electrocatalysts for applications in clean energy production. A hybrid electrocatalyst, synthesized from 2,10,16,24-tetrakis{4-((2-benzhydrylamino)phenyl)amino-2-isocyanobenzonitrile}cobalt phthalocyanine (CoTBPc) supported on Ketjen Black (KB), was prepared and comprehensively characterized using FTIR, NMR, Raman, UV-vis, SEM-EDS, and XPS analyses and other analytical methods. The CoTBPc + KB composite exhibits excellent hydrogen evolution reaction (HER) activity, with an overpotential of 229 mV at 10 mA cm<small>⁻²</small> in 1.0 M KOH. For the oxygen evolution reaction (OER), it shows an overpotential of 289 mV, demonstrating balanced bifunctional catalytic performance. The conductive KB framework facilitates rapid electron transfer and optimally exposes Co–N4 active sites. The catalyst also retains excellent operational stability for 47 hours (HER) and 52 hours (OER) during continuous electrolysis. These outcomes make CoTBPc + KB a durable and promising candidate for alkaline water-splitting applications.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 9","pages":" 2344-2354"},"PeriodicalIF":4.1,"publicationDate":"2026-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147826926","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Discussion on the mechanism of the electrocatalytic reduction of furfural using thermodynamic, voltammetry, and simulation methods","authors":"Yiming Cui, Ze Wang, Jie Hao, Xiaoxia Li and Songgeng Li","doi":"10.1039/D5SE01645B","DOIUrl":"https://doi.org/10.1039/D5SE01645B","url":null,"abstract":"<p >Electrocatalytic reduction (ECR) of bio-oil (from the pyrolysis of biomass) has attracted great attention because of its operation under ambient conditions and the use of water as a hydrogen donor. Furfural (FF) is an important component of bio-oil. 2-Methylfuran (2-MF) can be used as a gasoline antiknock agent. The ECR of FF to produce 2-MF is investigated. Low temperature is found to be favorable for the ECR of FF and disadvantageous for the formation of H<small>₂</small>. Ni has a higher activity than Cu. For Ni–Cu electrode, the reaction initiates as late as that on Cu, but the conversion becomes faster once reaction starts. A trace amount of Ni<small>²⁺</small> (10<small>⁻⁷</small> M) in the electrolyte has nearly no influence on the reaction overpotential but could improve the extent of conversion. The carbonyl bond of furfural is activated when the carbonyl O atom approaches the Cu atom and the carbonyl C atom is close to Ni.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 8","pages":" 2059-2069"},"PeriodicalIF":4.1,"publicationDate":"2026-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147727293","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Tannic acid-derived metal–phenolic networks with dual-atom ORR and single-atom OER sites for bifunctional oxygen electrocatalysts","authors":"Shilong Wen, Zhen Zhang and Xikui Liu","doi":"10.1039/D6SE00142D","DOIUrl":"https://doi.org/10.1039/D6SE00142D","url":null,"abstract":"<p >Developing highly efficient and cost-effective bifunctional oxygen electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is critical for the widespread application of rechargeable zinc–air batteries. Herein, we report a green-synthesized, tannic acid-derived metal–phenolic networks electrocatalyst featuring well-defined dual-atom ORR sites and single-atom OER sites, which synergistically deliver exceptional bifunctional activity. The unique structure originates from the precise coordination of earth-abundant metal ions with the polyphenol ligand of natural tannic acid, providing well-defined active sites and efficient mass/electron transport. The optimized catalyst Co<small>_0.85</small>Fe<small>_0.15</small>@TA-Salphen exhibits outstanding ORR performance with a half-wave potential of 0.923 V (<em>vs.</em> RHE) and superior OER activity with an overpotential of only 282 mV at 10 mA cm<small>⁻²</small>, surpassing most reported bifunctional catalysts. When integrated into zinc–air batteries, the catalyst demonstrates high power density (198 mW cm<small>⁻²</small>) and excellent cycling stability (over 500 cycles), highlighting its potential for practical applications. This work not only presents a high-performing and durable bifunctional oxygen electrocatalyst with well-defined ORR/OER active sites but also highlights the potential of green, biomass-derived materials for advanced energy applications.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 8","pages":" 2081-2089"},"PeriodicalIF":4.1,"publicationDate":"2026-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147727296","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Methane synthesis from CO2 and H2O with concentrated NaOH–KOH electrolyte at 200–250 °C using electrochemical Pd–Ag membrane reactor","authors":"Wakana Seki, Raisei Sagara, Aika Hirata and Jun Kubota","doi":"10.1039/D5SE01657F","DOIUrl":"https://doi.org/10.1039/D5SE01657F","url":null,"abstract":"<p >The synthesis of hydrocarbons from CO<small>₂</small> and H<small>₂</small>O using electricity derived from renewable energy sources has attracted considerable attention. However, there is currently no direct electrochemical method capable of selectively producing specific hydrocarbons from CO<small>₂</small> reduction at low overpotentials. By employing an electrochemical membrane reactor that combines water electrolysis with thermocatalytic methanation, methane can be selectively produced at a cell voltage comparable to that of conventional water electrolysis. In this study, methane synthesis from CO<small>₂</small> and H<small>₂</small>O was investigated using an electrochemical membrane reactor equipped with a 30 wt%-Ru/C catalyst, Pd-based alloy membrane, and a NaOH–KOH eutectic electrolyte operating at approximately 250 °C. At 250 mA cm<small>⁻²</small> based on cathode geometric area and 250 °C, the methane and hydrogen production rate was 290 and 120 nmol s<small>⁻¹</small> cm<small>⁻²</small>, corresponding to a current efficiency of 91 and 9%, respectively. However, when the current density exceeded 250 mA cm<small>⁻²</small>, the total current efficiency suddenly deviated significantly from 100%, indicating a decrease in current efficiency due to product cross-leak. At 300 mA cm<small>⁻²</small>, significant evolution of H<small>₂</small> was detected in the anode-side exhaust gas. This cross-leak was also pronounced during operation below 200 °C. Impedance measurements determined that the specific resistance of the electrolyte at 250 °C was 0.50 S cm<small>⁻¹</small>. The current efficiency and related characteristics of this methane synthesis method were discussed in detail.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 8","pages":" 2070-2080"},"PeriodicalIF":4.1,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/se/d5se01657f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147727295","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Mitigating redox mediator-induced surface recombination for efficient photoelectrocatalytic benzyl alcohol oxidation on Mo-doped bismuth vanadate","authors":"Chun-Chung Kuang, Yi-Wen Chen, Guan-Zhu Tu, Hong-Lin Chen, Jun-Lin Fong, Yi-Sheng Wang, Chia-Wei Chang, Jing-Yan Wu, Ting-Ting Chang, Chao-Hsien Chang, Hong-Kang Tian and Chang-Ming Jiang","doi":"10.1039/D6SE00110F","DOIUrl":"https://doi.org/10.1039/D6SE00110F","url":null,"abstract":"<p >Synthetic photoelectrochemistry offers a sustainable route for selective organic transformations under visible light, yet carrier recombination losses at the electrode–electrolyte interfaces remain a critical bottleneck. Although redox mediators are often employed to improve selectivity and circumvent kinetic barriers, their interactions with the photoelectrodes are not well understood. Here we show that <em>N</em>-hydroxysuccinimide (NHS), a widely used hydrogen atom transfer (HAT) mediator, dynamically adsorbs onto oxygen vacancies on BiVO<small>₄</small> photoanodes, forming extrinsic interfacial states that trap photogenerated holes. Time-resolved photoelectrochemical and voltametric analyses reveal a direct correlation between this interfacial recombination pathway, photocurrent declines, and diminished reaction yields. Incorporating Mo dopant in BiVO<small>₄</small> increases the oxygen-vacancy formation energy, while electrolyte cation tuning modulates the electrochemical double-layer structure, jointly suppressing NHS chemisorption and mitigating surface recombination. During selective PEC oxidation of benzyl alcohol to benzaldehyde, optimized Mo-doped BiVO<small>₄</small> photoanodes achieve a conversion rate of 19.1 ± 1.4 µmol cm<small>⁻²</small> h<small>⁻¹</small> with &gt;92% faradaic efficiency, representing the highest performance reported for BiVO<small>₄</small>-based benzylic alcohol oxidation. These findings identify interfacial mediator adsorption as a previously overlooked recombination channel and establish rational interfacial design as a powerful strategy for broadly tunable, high-efficiency light-driven organic synthesis.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 8","pages":" 2090-2100"},"PeriodicalIF":4.1,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147727297","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Co2NiO4/NF as a bidirectional catalyst for quinoxaline hydrogenation/tetrahydroquinoxaline dehydrogenation in flow batteries","authors":"Fangcheng Qiu, Nan Wang, Bowen Chen, Xin Zheng, Hanyu Li, Xue Han, Shaowen Tan, Siyi Chen and Shengping Wang","doi":"10.1039/D6SE00166A","DOIUrl":"https://doi.org/10.1039/D6SE00166A","url":null,"abstract":"<p >This study addresses key challenges in conventional catalysis for the quinoxaline/tetrahydroquinoxaline liquid organic hydrogen carrier (LOHC) pair. These challenges include high energy consumption, reliance on precious metals, and catalyst irreversibility. We developed a novel strategy for fabricating an efficient bifunctional electrode. This strategy is based on electrodeposition from a deep eutectic ionic liquid. The Co–Ni bimetallic catalyst (Co<small>₂</small>NiO<small>₄</small>/NF) was constructed on a nickel foam (NF) substrate. This was achieved <em>via</em> electrodeposition in a choline chloride–propylene glycol ionic liquid. Physicochemical characterization confirmed the catalyst's unique structure. This structure is a composite of metallic cobalt and cobalt–nickel oxide. It also features uniformly distributed active sites. Electrochemical tests demonstrate high activity and selectivity for Co<small>₂</small>NiO<small>₄</small>/NF. It performs well in both the electrocatalytic hydrogenation of quinoxaline and the electrocatalytic dehydrogenation of tetrahydroquinoxaline. The catalyst also shows excellent cycling stability in both reactions. This enables efficient bidirectional catalysis for the reversible hydrogen storage and release processes of LOHCs on a single catalyst platform. Under optimal potentials, the faradaic efficiency reached 99.84% (with 98.73% selectivity) for hydrogenation. For dehydrogenation, it reached 99.07% (with 98.96% selectivity). The performance enhancement is attributed to the electronic synergy between Co and Ni. This synergy optimizes the electrode's conductivity and reactant adsorption behavior. Furthermore, the reversible valence cycling of the cobalt/nickel redox couple provides a distinct kinetic advantage, continuously facilitating both the hydrogenation and dehydrogenation processes. This work provides a new material system and design approach. It aids in the development of low-cost, high-performance bifunctional catalysts for LOHCs and also promotes progress toward the practical application of quinoxaline-based organic flow batteries.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 9","pages":" 2230-2244"},"PeriodicalIF":4.1,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147827000","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Thermophysical characterization of a new potential bio-oxygenate fuel formed by hexane, ethanol and diethyl carbonate","authors":"Ariel. Hernández, Marcela. Cartes and Andrés. Mejía","doi":"10.1039/D6SE00129G","DOIUrl":"https://doi.org/10.1039/D6SE00129G","url":null,"abstract":"<p >The thermophysical characterization of a new potential bio-oxygenate fuel formed by ethanol, diethyl carbonate, and hexane is carried out by the direct determinations and theoretical predictions of the selected fundamental thermophysical properties (<em>i.e.</em>, vapor–liquid equilibria, dynamic viscosity, and surface tension) over the entire mole fraction range. Specifically, vapor–liquid equilibria (VLE) are reported at 94.00 kPa, over 330.0 K to 356.0 K, while liquid dynamic viscosity and surface tension are explored at 298.15 K and 101.3 kPa. The experimental VLE are modeled using the Perturbed Chain Statistical Associating Fluid Theory Equation of State (PC-SAFT EoS), which accounts for hydrogen bonding interactions between alcohol molecules and cross-interactions with the negative sites on the diethyl carbonate molecule. For the other two reported properties, the PC-SAFT EoS is coupled with free-volume theory and linear gradient theory, respectively. The advantage of this combined approach is that all required parameters are obtained from the corresponding pure fluids and binary mixtures that form the ternary mixture; therefore, the thermophysical properties of the ternary mixture are completely predicted. Based on experimental determinations and theoretical modeling, the VLE of the ternary mixture exhibits a positive deviation from Raoult's law, indicating zeotropic behavior under the conditions explored. The dynamic viscosities and surface tension display a monotonic behavior with the mole fraction. Finally, the combination of experimental measurements and molecular-based theoretical model provides a reliable framework to predict with physical sound and good accuracy these thermophysical properties over a broad range of temperature, pressure, and mole fractions that can be safely used to carry out further evaluations related to the use of this oxygenate fuel in complementary engine tests.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 8","pages":" 1947-1958"},"PeriodicalIF":4.1,"publicationDate":"2026-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/se/d6se00129g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147727280","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Ionic liquid-engineered core–shell polymer nanospheres for photocatalytic nitrogen reduction","authors":"Ning Zhang, Dorian Priano, Catherine Santini, Jinlong Zhang and Stephane Daniele","doi":"10.1039/D5SE01680K","DOIUrl":"https://doi.org/10.1039/D5SE01680K","url":null,"abstract":"<p >Resorcinol–formaldehyde resin (RF), a novel organic photocatalytic material, has seen extensive application in the photocatalytic generation of hydrogen peroxide in recent years, owing to its broad band gap structure and robust visible light absorption capabilities. The favorable positions of the conduction and valence bands of RF theoretically enable RF application in photocatalytic nitrogen fixation. Nevertheless, the limited solubility of nitrogen in water results in diminishing the effectiveness of photocatalytic nitrogen fixation. Herein, we present a method to coat RF nanospheres with an ionic liquid (RF@IL) exhibiting significant nitrogen enrichment capacity to develop a novel organic semiconductor material featuring a core–shell configuration. The abundant hydroxyl functional groups on the surface of RF nanospheres facilitate the coating of imidazolium ionic liquids, affording a nitrogen-rich thin film for the RF nanospheres and segregate the sites of nitrogen reduction and water oxidation, minimizing the recombination of photogenerated carriers and thereby enhancing the efficacy of the photocatalytic nitrogen fixation reaction. RF@IL facilitated photocatalytic nitrogen fixation, yielding 58.7 µmol g<small>⁻¹</small> of ammonia in 2 hours, which is 1.80 times greater than the blank RF output of 32.6 µmol g<small>⁻¹</small>. Remarkably, after five testing cycles, RF@IL retains substantial photocatalytic ammonia synthesis activity, underscoring the considerable influence of ionic liquids on photocatalytic processes. This study offers a viable solution to the issue of low nitrogen solubility impacting reaction performance in photocatalytic nitrogen fixation experiments.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 9","pages":" 2245-2255"},"PeriodicalIF":4.1,"publicationDate":"2026-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/se/d5se01680k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147826919","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Photophysical reappraisal of additives for photovoltaic systems: a case study on three hole transporting materials and two dopants","authors":"Sergio Ramírez-Barroso, Jorge Marco-Guimbao, David García-Fresnadillo, Nazario Martín and Juan Luis Delgado","doi":"10.1039/D6SE00274A","DOIUrl":"https://doi.org/10.1039/D6SE00274A","url":null,"abstract":"<p >A study on the dissimilar interactions of two photovoltaic additives, <strong>FK209</strong> or a combination of <strong>LiTFSI</strong> and <strong>TBP</strong> dopants, with three structurally different molecular hole-transporting materials (HTMs) previously used in perovskite solar cells (PSCs) is presented. The investigated HTMs are <strong>Spiro-OMeTAD</strong> and a toroidally delocalized oligotriarylamine-hexaarylbenzene derivative (<strong>HAB1</strong>), both globular and structurally rigid, as well as a globular but structurally fluxional oligotriarylamine-[60]fullerene hexakis-adduct (<strong>FU7</strong>). Photophysical characterisation with/without the additives in solution has been performed considering the changes in UV-vis absorption and fluorescence excitation/emission spectra of the HTMs, modulation of their emission quantum yields and lifetimes, analysis of the excited state quenching by the dopants, results of time-resolved fluorescence anisotropy assays accounting for changes in the size of the HTMs behaving as fluorophores, and evaluation of the singlet oxygen production by the HTMs. <strong>FK209</strong> efficiently promotes charge transfer by association with the molecular HTMs, as evidenced by the observation of static quenching and variations of their rotational lifetimes due to increased fluorophore sizes; the charge transfer process with the <strong>LiTFSI</strong> and <strong>TBP</strong> system is only based on diffusion-controlled dynamic quenching of the excited HTMs, suggesting a weaker interaction, which is modulated by the accessibility of small hydrophobic molecules such as <strong>LiTFSI</strong> and <strong>TBP</strong> to the inner domains of the molecular HTMs. Remarkably, <strong>Spiro-OMeTAD</strong> shows competitive singlet oxygen photosensitisation by energy transfer, with a non-negligible quantum yield of 0.35. This study shows excellent agreement with previously reported results in PSCs, providing a better understanding of the underlying interactions between HTMs and dopants and, in turn, facilitating the optimisation of decisions regarding additives employed in photovoltaic devices.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 9","pages":" 2196-2208"},"PeriodicalIF":4.1,"publicationDate":"2026-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147826997","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}