{"title":"Ammonia synthesis from water and nitrogen using electricity with a hydrogen-permeable membrane electrochemical cell with Ru catalysts and molten hydroxide electrolyte: integration with ammonia separation and unreacted gas recirculation†","authors":"Raisei Sagara, Eriko Watanabe and Jun Kubota","doi":"10.1039/D5SE00348B","DOIUrl":"https://doi.org/10.1039/D5SE00348B","url":null,"abstract":"<p >There is considerable interest in synthesizing NH<small><sub>3</sub></small> directly from abundant H<small><sub>2</sub></small>O and N<small><sub>2</sub></small> using electricity from renewable energy sources, for applications such as synthetic fuels, artificial fertilizers, and raw materials for plastics. NH<small><sub>3</sub></small> synthesis from N<small><sub>2</sub></small> and H<small><sub>2</sub></small>O was investigated using an electrochemical setup featuring Ru/Cs<small><sup>+</sup></small>/C catalysts, Pd alloy membrane cathodes, NaOH–KOH molten electrolytes, and Ni anodes operated at 250 °C and 1.0 MPa (absolute). This electrochemical setup was integrated with a refrigerated gas/liquid separator at −75 °C to concentrate NH<small><sub>3</sub></small> and a recirculation pump for unreacted H<small><sub>2</sub></small> and N<small><sub>2</sub></small>. As a single-pass reactor, if NH<small><sub>3</sub></small> separation and unreacted gas recirculation were not used, this electrochemical device produced NH<small><sub>3</sub></small> at 1.0 MPa and 250 °C, with an apparent current efficiency of 32–20% at 10–100 mA cm<small><sup>−2</sup></small>. This efficiency was limited by the chemical equilibrium, which is calculated to be 36%. The study achieved a 90% apparent current efficiency, with a 320 nmol s<small><sup>−1</sup></small> cm<small><sup>−2</sup></small> production rate of NH<small><sub>3</sub></small> at 100 mA cm<small><sup>−2</sup></small>, 250 °C, and 1.0 MPa with NH<small><sub>3</sub></small> separation and unreacted gas recirculation. The remaining 10% of the apparent current efficiency was used for H<small><sub>2</sub></small> production. The reaction kinetic properties and scalability of the present system were discussed.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 10","pages":" 2658-2669"},"PeriodicalIF":5.0,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/se/d5se00348b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143944164","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":"Efficient and durable perovskite photovoltaics using dibenzothiophene arylamine derivatives for indoor energy harvesting†","authors":"Lal Chand, Prasun Kumar, Rahul Tiwari, Babar Suraj Shivaji, Milon Kundar, Suman Kalyan Pal, Vibha Saxena, Ranbir Singh and Surya Prakash Singh","doi":"10.1039/D5SE00293A","DOIUrl":"https://doi.org/10.1039/D5SE00293A","url":null,"abstract":"<p >Developing efficient and stable hole-transporting materials (HTMs) is critical for improving the performance of perovskite photovoltaic (PPV) devices, especially for indoor applications. Herein, we introduce two novel dibenzothiophene-based small organic molecule HTMs, labelled <strong>DBT-1</strong> and <strong>DBT-2</strong>. These HTMs, featuring DBT as an acceptor and methoxy-substituted diphenylamine as a donor group, were designed to improve PPV devices' stability, charge transport properties, and efficiency. Theoretical studies confirmed the distinct geometries of the HTMs, revealing a more delocalized electron distribution in <strong>DBT-2</strong> than in <strong>DBT-1</strong>, resulting in enhanced electronic properties. Optoelectronic properties revealed that both HTMs have higher highest occupied molecular orbital (HOMO) energy levels than perovskite, ensuring efficient hole extraction. When integrated into indoor perovskite photovoltaic (IPPV) devices, the <strong>DBT-2</strong> HTM achieved a remarkable power conversion efficiency (PCE) of 33.32% under 1000 lux LED lighting, outperforming <strong>Spiro-OMeTAD</strong>-based devices by 28.13%. Notably, the hydrophobic nature and uniform film morphology of <strong>DBT-2</strong> contributed to enhanced stability. Furthermore, after 200 hours of thermal stress at 80 °C, both HTMs demonstrated outstanding thermal stability, maintaining 91% of their initial efficiency. These results indicate that <strong>DBT-2</strong> is a promising dopant-free HTM for efficient, reliable, and cost-effective PPVs, particularly in indoor applications. The high performance and durability of these materials make them strong contenders for next-generation indoor photovoltaic applications.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 11","pages":" 2993-3003"},"PeriodicalIF":5.0,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144148181","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}
Hálfdán Ingi Gunnarsson, Naveed Ashraf and Younes Abghoui
{"title":"Analyses of vanadium carbide as an anode for post-lithium batteries","authors":"Hálfdán Ingi Gunnarsson, Naveed Ashraf and Younes Abghoui","doi":"10.1039/D5SE00193E","DOIUrl":"https://doi.org/10.1039/D5SE00193E","url":null,"abstract":"<p >Today, lithium batteries dominate the market of rechargeable batteries, but lithium production is expensive and environmentally detrimental. Given increasing demand and rising costs, the search for alternative rechargeable batteries is critical. This work investigates the performance of a promising 2D MXene anode material, vanadium carbide (V<small><sub>2</sub></small>C), for use in metal-ion batteries. We compare the properties of four promising alternative metal-ions (Na, Mg, Al, and Ag) with lithium (Li) using DFT. The comparison revealed that Na and Ag perform comparably to Li, with a respective OCV of 0.66–1.32 V and 0.91–1.23 V, with respective theoretical specific capacities of 627 mA h g<small><sup>−1</sup></small> and 967 mA h g<small><sup>−1</sup></small>, compared to an OCV of 0.75–1.00 V and a capacity of 967 mA h g<small><sup>−1</sup></small> for Li. The diffusive barrier of Na is exceptionally low, 0.007 eV, and the barrier for Ag is 0.07 eV, while the barrier for Li is 0.02 eV. The Mg- and Al-ion batteries perform with a very high maximum charging capacity, 1883 mA h g<small><sup>−1</sup></small> and 2823 mA h g<small><sup>−1</sup></small> respectively, and a slightly lower OCV range of 0.39–0.45 V and 0.22–0.45 V respectively. Due to the good capacity, high OCV and low diffusive barriers of the ions, V<small><sub>2</sub></small>C anodes are ideal for post-lithium metal-ion battery applications.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 11","pages":" 3068-3077"},"PeriodicalIF":5.0,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144148206","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}
Jin Yan, Jasmeen Nespoli, Reinder K. Boekhoff, Haoxu Wang, Timo Gort, Martijn Tijssen, Bernardus Zijlstra, Arjan Houtepen, Tom J. Savenije, Olindo Isabella and Luana Mazzarella
{"title":"Chloride-improved crystallization in sequentially vacuum-deposited perovskites for p–i–n perovskite solar cells†","authors":"Jin Yan, Jasmeen Nespoli, Reinder K. Boekhoff, Haoxu Wang, Timo Gort, Martijn Tijssen, Bernardus Zijlstra, Arjan Houtepen, Tom J. Savenije, Olindo Isabella and Luana Mazzarella","doi":"10.1039/D4SE01744G","DOIUrl":"https://doi.org/10.1039/D4SE01744G","url":null,"abstract":"<p >Sequential thermal evaporation is an emerging technique for obtaining perovskite (PVK) photoactive materials for solar cell applications. Advantages include solvent-free processing, accurate stoichiometry control, and scalable processing. Nevertheless, the power conversion efficiency (PCE) of PVK solar cells (PSCs) fabricated by evaporation still lags behind that of solution-processed PSCs. Here, based on multi-cycle sequential thermal evaporation, we systematically investigate the effects of the post-deposition annealing temperature on the PVK properties in terms of surface morphology, opto-electronic properties, and device performance. We find that the average grain size increases to almost 1 μm and charge carrier mobilities exceed 50 cm<small><sup>2</sup></small> V<small><sup>−1</sup></small> s<small><sup>−1</sup></small> when the annealing temperature is increased to 170 °C. We introduce a trace of PbCl<small><sub>2</sub></small> to the multi-cycle sequential deposition to improve the absorber crystallinity at a lower annealing temperature of 150 °C, as evidenced by the XRD and PL analyses. The resulting PSC in a p–i–n structure yields a PCE of 18.5% with a cell area of 0.09 cm<small><sup>2</sup></small>. With the same deposition parameters, the cell area is scaled up to 0.36 cm<small><sup>2</sup></small>, achieving champion PCEs of 17.06%. This indicates the great potential of this technology for the commercialization of PSCs in the future.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 10","pages":" 2729-2737"},"PeriodicalIF":5.0,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/se/d4se01744g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143943991","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}
Shambhulinga Aralekallu, Lokesh Koodlur Sannegowda, Mahaveer D. Kurkuri, Ranjith Krishna Pai and Ho-Young Jung
{"title":"Hybrid water electrolysis as the way forward to sustainable hydrogen production","authors":"Shambhulinga Aralekallu, Lokesh Koodlur Sannegowda, Mahaveer D. Kurkuri, Ranjith Krishna Pai and Ho-Young Jung","doi":"10.1039/D5SE00236B","DOIUrl":"https://doi.org/10.1039/D5SE00236B","url":null,"abstract":"<p >Replacing the anodic oxygen evolution reaction (OER) with energy saving and more favorable electrochemical oxidation reactions opens a new door to an innovative way for sustainable hydrogen production. Specifically, the electro-oxidation of organic compounds, biomass molecules, and plastic waste has attracted tremendous interest in recent years owing to its potential for H<small><sub>2</sub></small> production at the cathode chamber and production of value-added chemicals and fuels at the anode chamber. This review is not intended to provide an in-depth, comprehensive overview of all these reactions and hybrid water electrolysis but rather highlight the key aspects of hybrid water electrolysis. The basic understanding of hybrid water electrolysis, its advantages over conventional water electrolysis, major reactions, bifunctional electrocatalysts and their fabrication based on the available information are discussed. Although this review sheds light on the basic understanding of alternative oxidation reactions in hybrid water electrolysis, a special focus is given on the important question of whether the bifunctional electrocatalysts employed in conventional water electrolysis will be effective in hybrid water electrolysis. Lastly, the challenges and perspectives are discussed.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 11","pages":" 2928-2940"},"PeriodicalIF":5.0,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144148282","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":"Environmentally sustainable fabrication of organic solar cells: preserving the power conversion efficiency while reducing the material footprint†","authors":"Ushasri Mukherjee and Samarendra P. Singh","doi":"10.1039/D5SE00413F","DOIUrl":"https://doi.org/10.1039/D5SE00413F","url":null,"abstract":"<p >Organic solar cells (OSCs) have attracted significant interest due to their utilization of a solution-based approach, which allows for easier fabrication procedures. In recent years, OSCs have successfully reached more than 19.0% of power conversion efficiency (PCE). Most of these interesting developments commonly utilized halogenated solvents such as chlorobenzene (CB), chloroform (CF), 1,2-dichlorobenzene (ODCB), <em>etc</em>. These halogenated solvents are harmful to human health as well as the environment. Therefore, the utilization of harmful solvents limits its capability as an environmentally friendly technology. With an aim to employ eco-friendly solvents for OSC fabrication, we present our research on the fabrication of PTB7-Th:PC<small><sub>71</sub></small>BM-based organic solar cells (OSCs) using a combination of non-halogenated and relatively eco-friendly solvents. The combination of 2-methylanisole (MA) and mesitylene (MY) in a specific ratio (7 : 3) has been identified as a suitable substitute solvent. By employing these solvents, we were able to reach a maximum PCE of 7.32% for the OSCs with an inverted device architecture ITO/ZnO/PTB7-Th:PC<small><sub>71</sub></small>BM/MoO<small><sub><em>x</em></sub></small>/Ag, which is comparable to the PCE of OSCs processed using ODCB solvent. Furthermore, we established the universality of a relatively non-toxic solvent combination (MA : MY) for eco-friendly OSCs by achieving a PCE of 11.05% for the ternary device architecture ITO/ZnO/PTB7-Th:Y7:IT-M/MoO<small><sub><em>x</em></sub></small>/Ag.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 10","pages":" 2792-2804"},"PeriodicalIF":5.0,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143944001","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":"Strong impacts of inter-π-chain charge transfer accelerating CO2 reduction photocatalysis of carbazole–diimine-based linear conjugated polymer/Ru complex hybrids†","authors":"Akinobu Nakada, Shunsuke Asai, Chen Zhang, Kotaro Ishihara, Hajime Suzuki, Osamu Tomita, Katsuaki Suzuki, Hironori Kaji, Akinori Saeki and Ryu Abe","doi":"10.1039/D5SE00142K","DOIUrl":"https://doi.org/10.1039/D5SE00142K","url":null,"abstract":"<p >Conjugated polymers are promising candidates for photocatalyst materials owing to the molecular design flexibility in tuning their properties, including visible light responsiveness. The rational introduction of a molecular metal complex acting as a catalyst at a specific location is an effective approach to activate conjugated polymer photocatalysts for the selective conversion of small molecules, such as carbon dioxide. However, the photocatalytic activity of the conjugated polymer/metal complex hybrids has not been satisfactory. In particular, there is still much room for improvement in polymer structure engineering to maximise the activation of a molecular complex catalyst centre by photoexcited electrons. This work demonstrates the strong impact of side chains and ligand structures, which do not significantly affect the optical properties of the polymers, on their photocatalytic performance for CO<small><sub>2</sub></small> reduction. The relatively rigid aromatic side chains and condensed aromatic ligand moieties enable effective inter-π-chain charge transfer to activate the isolated (<em>i.e.</em> low-concentration) Ru(<small>II</small>) complex catalyst. The manipulation of photoexcited charge transfer by structural modulation resulted in a significantly improved photocatalytic activity (quantum efficiency of 2.2% at 450 nm) compared to the counterpart photocatalysts containing the alkyl side chain and bipyridine ligand moieties.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 11","pages":" 2941-2950"},"PeriodicalIF":5.0,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/se/d5se00142k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144148283","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":"Additive passivation strategies to improve properties of evaporation-spray coating perovskite solar cells†","authors":"Yuxin Zhang, Cong Geng, Chunyang Zheng, Huiren Zheng, Xin Zhao, Mingwei Zhu, Yong Peng and Yi-Bing Cheng","doi":"10.1039/D5SE00143A","DOIUrl":"https://doi.org/10.1039/D5SE00143A","url":null,"abstract":"<p >The evaporation-spray coating process has been applied in the field of perovskites. However, perovskite solar cells fabricated using the evaporation-spray coating process often exhibit significant hysteresis, which is attributed to the ease of ion migration and interface recombination in the perovskite produced by this method. To address this issue, we introduced butylamine additives containing different halide ions (I<small><sup>−</sup></small>, Br<small><sup>−</sup></small>, Cl<small><sup>−</sup></small>) into the spray process. After comparing the results, it was found that butylamine iodide (BAI) can effectively passivate lead and iodide-related defects in the perovskite by interacting with uncoordinated lead and iodide ions, thereby suppressing non-radiative recombination. Additionally, BAI promotes the transformation of PbI<small><sub>2</sub></small> during the evaporation-spray coating process, reducing the residual lead iodide in the perovskite. The wide-bandgap perovskite solar cells (energy gap (<em>E</em><small><sub>g</sub></small>), <em>E</em><small><sub>g</sub></small> ≈ 1.68 eV) fabricated using this method achieved a champion device photovoltaic conversion efficiency (PCE) increase from 16.61% to 19.91%. Furthermore, the unencapsulated devices demonstrated excellent stability, maintaining 80% of their initial efficiency after 450 hours of thermal aging at 60 °C.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 10","pages":" 2670-2677"},"PeriodicalIF":5.0,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143944165","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":"Ultra-low loading porphyrin-incorporated conjugated polymer dots as photocatalysts for aerobic oxidation of sulfides in water†","authors":"Wissuta Boonta, Ratanakorn Teerasarunyanon, Chattarika Sukpattanacharoen, Sanhawat Rumporee, Phurinat Lorwongkamol, Nattapong Paiboonvorachat, Pongphak Chidchob, Suwit Suthirakun and Junjuda Unruangsri","doi":"10.1039/D5SE00146C","DOIUrl":"https://doi.org/10.1039/D5SE00146C","url":null,"abstract":"<p >The development of metal-free, low-loading catalysts, together with the use of water as a benign solvent is desirable for advancing facile and efficient catalysis of organic transformations in an environmentally friendly manner. The direct oxidation of sulfides to sulfoxides is a key process in organic synthesis and pharmaceuticals. This study introduces metal-free porphyrin-integrated poly[9,9′-dioctylfluorenyl-2,7-diyl)-<em>co</em>-(1,4-benzo-thiadiazole)] polymer dots (<strong>PFBT-TPP Pdots</strong>) as photocatalysts for photo-aerobic sulfide oxidation in water. <strong>PFBT-TPP Pdots</strong> were synthesized by the Suzuki–Miyaura cross-coupling process. DFT calculations confirmed the conjugation and delocalization characteristics of TPP incorporated into <strong>PFBT</strong>. The conjugated polymers were converted into Pdots using coprecipitation with poly(styrene-<em>co</em>-maleic anhydride). Pdots with a diameter of around 30 nm demonstrated exceptional dispersion in water. <strong>PFBT-TPP Pdots</strong> efficiently photocatalyzed 0.1 M of thioanisole or other sulfide derivatives, attaining remarkable conversion efficiency (80–100%) and selectivity (88–100%) at a low catalytic loading (50 μg of conjugated polymer) in water, under 1 atm O<small><sub>2</sub></small>, at ambient temperature, and under 3 h-LED illumination (20 W, <em>λ</em> = 456 nm). The photocatalytic process was scaled to produce gram quantities of the isolated product with high selectivity and no signs of over-oxidation. This demonstrates a sustained and practical application. The computational analysis and experimental findings illustrated that <strong>PFBT-TPP Pdots</strong> effectively generated reactive oxygen species during photocatalysis, leading to enhanced catalytic efficiency compared to <strong>PFBT Pdots</strong> and their metal-containing counterparts. This study highlights the potential of Pdots for efficient, selective photocatalysis in aqueous environments, overcoming common solubility challenges for substrates and products.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 12","pages":" 3237-3247"},"PeriodicalIF":5.0,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144244063","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}
Vighneshwar Ganesh Bhat, Kavya S. Keremane, Subramanya K. S., Archana S., Akash Hegde, Ivy M. Asuo, Bed Poudel and Udaya Kumar Dalimba
{"title":"Dopant-free hydrophobic fluorene-based hole transport materials: impact of methoxy-substituted triphenylamine and carbazole peripheral groups on the performance of perovskite solar cells†","authors":"Vighneshwar Ganesh Bhat, Kavya S. Keremane, Subramanya K. S., Archana S., Akash Hegde, Ivy M. Asuo, Bed Poudel and Udaya Kumar Dalimba","doi":"10.1039/D5SE00120J","DOIUrl":"https://doi.org/10.1039/D5SE00120J","url":null,"abstract":"<p >Hole-transporting materials (HTMs) are crucial for charge separation in perovskite solar cells (PVSCs). Besides possessing suitable HOMO/LUMO energies, HTMs should ideally be hydrophobic to protect the perovskites from atmospheric moisture to enhance device stability. We designed two fluorene-core D–π–D-type organic HTMs (<strong>V1</strong> and <strong>V2</strong>), consisting of either 4,4′-methoxy triphenylamine (<strong>V1</strong>) or <em>N</em>-phenyl-3,6-methoxy carbazole (<strong>V2</strong>) as the peripheral donor moiety. Optoelectronic characterization and density functional theory calculations confirmed the intramolecular charge transfer within these new HTMs. UPS and REELS analyses revealed favorable HOMO–LUMO energy level alignment of <strong>V1</strong> and <strong>V2</strong> with the work functions of MAPbI<small><sub>3</sub></small> and gold electrode for effective charge extraction. TRPL and transient absorption studies commendably explained better quenching of perovskite's luminescence by <strong>V1</strong> over <strong>V2</strong>, suggesting a better interfacial contact of <strong>V1</strong> with the perovskite layer. Accordingly, the PVSCs with <strong>V1</strong> and <strong>V2</strong> as HTMs in an architecture ITO/SnO<small><sub>2</sub></small>/MAPbI<small><sub>3</sub></small>/HTM(<strong>V1</strong> or <strong>V2</strong>)/Au demonstrated power conversion efficiency (PCE) of 14.05% and 12.73% respectively. Also, the device with <strong>V1</strong> retains 75% of its initial efficiency for more than 480 hours. The contact angle measurements revealed the strong hydrophobicity of both alkylated fluorene molecules (<strong>V1</strong> and <strong>V2</strong>), and impedance spectroscopy measurements further revealed higher <em>R</em><small><sub>rec</sub></small> values for these HTMs, indicating improved charge transport and reduced recombination losses. These findings demonstrate the potential of the newly developed hydrophobic fluorene-based HTMs for achieving long-lasting performance in PVSCs.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 10","pages":" 2769-2781"},"PeriodicalIF":5.0,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143943999","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}