ACS Energy Letters 最新文献_第10页

Ion-Regulated Interfacial Solvation Enables Ether Electrolytes for 4.4 V Lithium Metal Batteries 离子调节界面溶剂化使4.4 V锂金属电池的醚电解质成为可能

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-30 DOI: 10.1021/acsenergylett.6c01870

Meinan Zhao, Kaixiang Ren, Qi Yu, Liang Li, Xinchun Song, Shilin Wu, Zihan Xu, Yongkang Zhang, Kepeng Bao, Zhipeng Jiang, Yongtao Li

{"title":"Ion-Regulated Interfacial Solvation Enables Ether Electrolytes for 4.4 V Lithium Metal Batteries","authors":"Meinan Zhao, Kaixiang Ren, Qi Yu, Liang Li, Xinchun Song, Shilin Wu, Zihan Xu, Yongkang Zhang, Kepeng Bao, Zhipeng Jiang, Yongtao Li","doi":"10.1021/acsenergylett.6c01870","DOIUrl":"10.1021/acsenergylett.6c01870","url":null,"abstract":"Lithium metal batteries (LMBs) require electrolytes that stabilize both lithium metal anodes (LMAs) and cathodes. Conventional strategies mainly reconstruct bulk solvation structures, often perturbing the intrinsic properties of the electrolyte. Here, we introduce an ion-regulated strategy to selectively tailor interfacial solvation structures (ISS). Surface-enhanced Raman spectroscopy (SERS) reveals cation-dominated solvation at the anode and anion-dominated solvation at the cathode. Accordingly, K+ and BH4– are employed as ionic regulators to modulate DME coordination and suppress interfacial decomposition. Adding only 0.05 M KBH4 enables reversible Li plating/stripping for 160 cycles at 3 mA cm–2 and 1 mAh cm–2 and increases the oxidation onset potential to 5.00 V. Li–LiNi0.8Co0.1Mn0.1O2 (NCM811) full cells retain 85.7% capacity after 100 cycles with a 20 mg cm–2 cathode, 50 μm Li, and a 4.4 V cutoff. These findings demonstrate that manipulating electrode-specific interfacial solvation provides a distinct route toward ether electrolytes for 4.4 V LMBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6641–6650"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091005","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Ion Association Dynamics Governs Low-Temperature Ion Transport of Sodium-Ion Battery Electrolytes 离子缔合动力学控制钠离子电池电解质的低温离子输运

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-10-01 DOI: 10.1021/acsenergylett.6c02269

Qi Qin, Jiale Liu, Bokang Xiao, Le Yang, Shuaikai Xu, Sheng Bi, Liang Zeng, Tangming Mo

{"title":"Ion Association Dynamics Governs Low-Temperature Ion Transport of Sodium-Ion Battery Electrolytes","authors":"Qi Qin, Jiale Liu, Bokang Xiao, Le Yang, Shuaikai Xu, Sheng Bi, Liang Zeng, Tangming Mo","doi":"10.1021/acsenergylett.6c02269","DOIUrl":"10.1021/acsenergylett.6c02269","url":null,"abstract":"Sodium-ion batteries (SIBs) are being explored for low-temperature energy storage, yet the molecular origin of severe ion-transport degradation upon cooling remains unclear. Here, we combine machine-learned molecular dynamics with in situ variable-temperature Raman spectroscopy to establish a quantitative static-dynamic framework that directly correlates Na+-solvent coordination, ion association, and ion transport in the organic electrolytes of sodium-ion batteries. Quantitative structural analysis reveals only modest changes in Na+-solvent coordination upon cooling, while solvent-separated ion pairs remain the most mobile transport species throughout the investigated temperature range. Instead, cooling only slightly increases the populations of ion association but markedly prolongs their lifetimes and suppresses their dynamic reorganization, progressively reducing the fraction of rapidly migrating Na+ ions and thereby accounting for the pronounced decline in electrolyte conductivity at low temperatures. These findings identify ion-association dynamics, rather than static solvation structures, as the dominant molecular factor governing low-temperature ion transport.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6888–6896"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091852","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Treatment of Perovskite Solar Cells by Complementary Cyclic Ammonium Agents 互补环铵剂处理钙钛矿型太阳能电池

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-10-01 DOI: 10.1021/acsenergylett.6c02119

Zihao Li, Mengjia Li, Stefania Cacovich, Antoine Seyeux, Javid Hajhemati, Tommaso Raimondi, Baptiste Bérenguier, Philip Schulz, José Alvarez, Cong Chen, Thierry Pauporté

{"title":"Treatment of Perovskite Solar Cells by Complementary Cyclic Ammonium Agents","authors":"Zihao Li, Mengjia Li, Stefania Cacovich, Antoine Seyeux, Javid Hajhemati, Tommaso Raimondi, Baptiste Bérenguier, Philip Schulz, José Alvarez, Cong Chen, Thierry Pauporté","doi":"10.1021/acsenergylett.6c02119","DOIUrl":"10.1021/acsenergylett.6c02119","url":null,"abstract":"Interfacial defect heterogeneity and insufficient passivation are major sources of nonradiative recombination losses in perovskite solar cells (PSCs). They not only increase carrier recombination but also perturb local band alignment. Here, a complementary cyclic ammonium passivation strategy mixing conjugated and nonconjugated agents is developed to simultaneously achieve homogeneous defect passivation and interface optimization in inverted PSCs. Especially, by combining piperazinium diiodide and 2-thiophenemethylammonium iodide, a synergistic passivation architecture is established that effectively homogenizes the interfacial electrostatic landscape while mixing passivating functional groups. Quasi-Fermi level splitting (QFLS) analysis combined with spatially resolved surface photovoltage (SPV) characterizations reveal that piperazine-dependent Voc losses originate from heterogeneous SPV distributions, whereas the complementary passivation strategy produces a highly uniform and enhanced SPV response across the perovskite film. The resulting uniform electrostatic environment suppresses nonradiative recombination, reduces the QFLS-VOC mismatch, and promotes efficient charge extraction. This strategy leads to stable PSC with a champion power conversion efficiency (PCE) of 27.18% with a certified steady-state PCE of 26.47%.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6793–6800"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149092280","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

An Amphiphilic Proton Donor Decouples Acidity from Interfacial Reactivity for Lithium-Mediated Ammonia Synthesis 一种两亲性质子供体将酸性从锂介导的氨合成的界面反应活性中解耦

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2026-10-07 DOI: 10.1021/acsenergylett.6c02477

Yeongbae Jeon,Shihyun Kim,Seong Hyeon Kweon,Bongseok Kim,Ahee Choi,Hyun Ji An,Seungwon Chung,Dongjun Kim,Sang Kyu Kwak,Jungwon Park,Yun Jeong Hwang

{"title":"An Amphiphilic Proton Donor Decouples Acidity from Interfacial Reactivity for Lithium-Mediated Ammonia Synthesis","authors":"Yeongbae Jeon,Shihyun Kim,Seong Hyeon Kweon,Bongseok Kim,Ahee Choi,Hyun Ji An,Seungwon Chung,Dongjun Kim,Sang Kyu Kwak,Jungwon Park,Yun Jeong Hwang","doi":"10.1021/acsenergylett.6c02477","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02477","url":null,"abstract":"Abstract Electrochemical ammonia synthesis via a lithium-mediated nitrogen reduction reaction (Li-NRR) faces a fundamental selectivity challenge in which proton donors that accelerate productive protonation simultaneously promote parasitic hydrogen evolution. Here, we demonstrate that 2,2,2-trifluoroethanol (TFE), an amphiphilic alcohol, mitigates this limitation by decoupling thermodynamic acidity from kinetic reactivity. Despite its high acidity, TFE suppresses parasitic reactions through rapid interfacial passivation associated with its fluorinated structure, while modulating the microstructure of a fluoride-rich solid electrolyte interphase (SEI). Blending TFE with ethanol further optimizes proton activity and hydrogen bonding, yielding a thin, uniform SEI enriched in highly crystalline LiF with reduced interfacial resistance. The optimized electrolyte achieved a Faradaic efficiency of 59.0% in a continuous-flow reactor, maintained stable performance under potential-cycling, and reached 82.8% in a high-pressure batch reactor. This study highlights proton-donor engineering as a key strategy to modulate the SEI nanostructure for selectivity in Li-NRR.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"59 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149151305","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Suppressing 2D Interfacial Reconstruction via Tetrafluoroborate Surface Engineering for Stable Perovskite Solar Cells 稳定钙钛矿太阳能电池的四氟硼酸盐表面工程抑制二维界面重建

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2026-10-07 DOI: 10.1021/acsenergylett.6c01987

Sanjay Sandhu,Zhenghong Xiong,Xin Liang,Nam-Gyu Park

{"title":"Suppressing 2D Interfacial Reconstruction via Tetrafluoroborate Surface Engineering for Stable Perovskite Solar Cells","authors":"Sanjay Sandhu,Zhenghong Xiong,Xin Liang,Nam-Gyu Park","doi":"10.1021/acsenergylett.6c01987","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c01987","url":null,"abstract":"Abstract Surface passivation using two-dimensional (2D) perovskites has been widely employed to improve the efficiency and stability of perovskite solar cells (PSCs). However, conventional 3D/2D heterointerfaces often suffer from interfacial reconstruction caused by spacer-cation migration during operation, leading to performance degradation. Here, we investigate pseudo-halogen-modified phenethylammonium salts (PEAX, X = SCN and BF4) for surface passivation. Unlike the commonly used phenethylammonium iodide (PEAI), which forms a low-dimensional interfacial phase, PEABF4 does not induce 2D perovskite formation but instead enables non-reconstructive surface passivation. PEABF4 treatment improves energy-level alignment, carrier lifetime, charge extraction, and crystallinity and suppresses surface traps and nonradiative recombination. As a result, PSCs achieve a power conversion efficiency of 24.72% with a VOC of 1.16 V, outperforming untreated and PEAI-treated devices. Furthermore, unencapsulated PEABF4-based devices retain 85.96% of their initial efficiency after 320 h of maximum power point tracking, demonstrating that pseudo-halogen engineering offers an effective route toward efficient and operationally stable PSCs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"41 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091718","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Thermodynamic Control of Excitation Transport Regimes in Nanocrystal Solids 纳米晶体固体中激发输运机制的热力学控制

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2026-10-06 DOI: 10.1021/acsenergylett.6c02596

Thomas B. Haward,Vincent J.-Y. Lim,Ihor Cherniukh,Joshua R. S. Lilly,Adam T. M. Wood,Maryna I. Bodnarchuk,Michael B. Johnston,Maksym V. Kovalenko,Laura M. Herz

{"title":"Thermodynamic Control of Excitation Transport Regimes in Nanocrystal Solids","authors":"Thomas B. Haward,Vincent J.-Y. Lim,Ihor Cherniukh,Joshua R. S. Lilly,Adam T. M. Wood,Maryna I. Bodnarchuk,Michael B. Johnston,Maksym V. Kovalenko,Laura M. Herz","doi":"10.1021/acsenergylett.6c02596","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02596","url":null,"abstract":"Abstract Controlling excitation transport is central to the operation of light-harvesting and light-emitting devices based on nanocrystal films. Exciton diffusion is typically described as hopping through a homogeneous medium; however, even highly monodisperse nanocrystal ensembles exhibit energetic disorder arising from size variation. We demonstrate that such disorder couples exciton diffusivity in real space to energetic relaxation within the density of states. Using spectrally and temporally resolved photoluminescence reabsorption spectroscopy of CsPbBr3 nanocrystal films, we separately track exciton diffusion and energetic relaxation across a range of temperatures and nanocrystal sizes. We find that at low temperature, excitons preferentially migrate downhill toward larger, lower-energy nanocrystals, causing a transient collapse of exciton diffusivity that is particularly pronounced for smaller nanocrystals exhibiting higher energetic disorder. At room temperature, these effects are effectively countered by thermally activated uphill transfer, restoring normal diffusion. Nanocrystal solids thus offer tunable transport properties governed by the interplay between disorder and thermal energy.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"2 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149092061","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Dynamic Solvent Participation Drives Sodium Storage in Oxygen Engineered Hard Carbon 动态溶剂参与驱动氧工程硬碳中钠的储存

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2026-10-06 DOI: 10.1021/acsenergylett.6c02029

Jian Cui,Panpan Su,Jie Zhang,Ruiyi Li,Zuoyi Xiao,Qingda An,Zhongwei Chen

引用次数: 0

Humidity-Regulated Wetting of Aqueous PEDOT:PSS Enables Surfactant-Free Hole-Transport Layers in Non-Fullerene-Based Inverted Organic Photovoltaics 水分PEDOT的湿度调节润湿：PSS在非富勒烯基倒置有机光伏中实现无表面活性剂的空穴传输层

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2026-10-06 DOI: 10.1021/acsenergylett.6c02028

Karin Iwa,Lulu Sun,Kazuma Nakajima,Ryota Fukuzawa,Shinjiro Umezu,Thuc-Quyen Nguyen,Daishi Inoue,Daisuke Hashizume,Sunghoon Lee,Kenjiro Fukuda,Takao Someya

{"title":"Humidity-Regulated Wetting of Aqueous PEDOT:PSS Enables Surfactant-Free Hole-Transport Layers in Non-Fullerene-Based Inverted Organic Photovoltaics","authors":"Karin Iwa,Lulu Sun,Kazuma Nakajima,Ryota Fukuzawa,Shinjiro Umezu,Thuc-Quyen Nguyen,Daishi Inoue,Daisuke Hashizume,Sunghoon Lee,Kenjiro Fukuda,Takao Someya","doi":"10.1021/acsenergylett.6c02028","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02028","url":null,"abstract":"Abstract Inverted organic photovoltaics (OPVs) feature operational stability; however, developing fully solution-processed devices remains challenging due to the poor wettability of PEDOT:PSS hole-transport layers (HTLs) on hydrophobic donor:acceptor bulk heterojunction active layers. Here, we demonstrate a surfactant-free, humidity-regulated spin-coating strategy for forming uniform PEDOT:PSS HTLs directly on PM6:Y6 active layers. By maintaining the relative humidity at 10% or lower during coating, continuous PEDOT:PSS films were obtained, enabling inverted OPVs with power conversion efficiency (PCE) above 14.5%. Furthermore, these devices retain over twice the PCE of molybdenum oxide-based devices after 100 h of light soaking under nitrogen. Bulk quantum efficiency analysis suggests that the acidic aqueous PEDOT:PSS dispersion may partially perturb the interface on the active layer, whereas it improves the overall device stability. This humidity-regulated coating approach provides a simple route toward solution-processable HTL integration in efficient and operationally stable inverted OPVs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"54 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091723","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Surface Passivation Suppresses α-Particle-Induced Trap Formation in Perovskite Solar Cells for Space Applications 空间应用钙钛矿太阳能电池表面钝化抑制α-粒子诱导的陷阱形成

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2026-10-05 DOI: 10.1021/acsenergylett.6c02610

Da Seul Lee,Hyeong Won Seo,Hyeji Han,Suwhan Kim,Suseong Jang,Sang Won Kang,Sungwon Cho,Seung Hyeon Chae,Donghan Kang,Nayeong Kwon,Nuri Na,Dong-Won Kang,Dohyung Kim,Jongchul Lim,Dong-Seok Kim,Jongsung Park

{"title":"Surface Passivation Suppresses α-Particle-Induced Trap Formation in Perovskite Solar Cells for Space Applications","authors":"Da Seul Lee,Hyeong Won Seo,Hyeji Han,Suwhan Kim,Suseong Jang,Sang Won Kang,Sungwon Cho,Seung Hyeon Chae,Donghan Kang,Nayeong Kwon,Nuri Na,Dong-Won Kang,Dohyung Kim,Jongchul Lim,Dong-Seok Kim,Jongsung Park","doi":"10.1021/acsenergylett.6c02610","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c02610","url":null,"abstract":"Abstract α-Particles represent the second most abundant ionic species in space radiation, yet their specific degradation mechanisms and mitigation strategies in perovskite solar cells (PSCs) remain unquantified. Here, we evaluate the degradation of PSCs under 2.5 MeV α-particle irradiation and investigate the protective role of a propane-1,3-diammonium iodide (PDAI2) surface passivation. Following irradiation, PDAI2-passivated target devices retain 80% of their initial efficiency (20.22%), whereas control devices retain 60% (19.13%). Performance losses were dominated by fill factor degradation. X-ray diffraction, scanning electron microscopy, and Fourier-transform infrared spectroscopy indicate that while α-particle induces partial organic cation loss and morphological variations, the primary crystalline phase is preserved without secondary phase decomposition. Capacitance–voltage, impedance spectroscopy, and Kelvin probe force microscopy confirmed that performance losses originate predominantly from photoactive trap states generated at the perovskite surface and interface, which increase space-charge density and transport resistance. Diammonium cations coordinate undercoordinated surface sites and crosslink organic cations, preventing radiation-generated point defects from stabilizing into transport-impeding traps. These findings establish surface defect chemistry control as a key strategy against high linear energy transfer (LET) ion radiation in space photovoltaics.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"9 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091722","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Wireless Monolithic Tandem Leaf for Semi-Artificial Photosynthesis 半人工光合作用的无线单片串联叶片

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2026-10-05 DOI: 10.1021/acsenergylett.6c01999

Minah Kim,Jihong Min,Chang Hyun Kim,Hyun-Woo Kim,Donggu Kim,Yire Han,Yonghoon Jung,Hanseul Choi,Hoyoung Song,Hyewon Park,Soo-Jin Yeom,Kwanyong Seo,Yun Seog Lee,Yoonmook Kang,Jeong Young Park,Byungha Shin,Chan Beum Park

{"title":"Wireless Monolithic Tandem Leaf for Semi-Artificial Photosynthesis","authors":"Minah Kim,Jihong Min,Chang Hyun Kim,Hyun-Woo Kim,Donggu Kim,Yire Han,Yonghoon Jung,Hanseul Choi,Hoyoung Song,Hyewon Park,Soo-Jin Yeom,Kwanyong Seo,Yun Seog Lee,Yoonmook Kang,Jeong Young Park,Byungha Shin,Chan Beum Park","doi":"10.1021/acsenergylett.6c01999","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c01999","url":null,"abstract":"Abstract Biocatalytic semi-artificial photosynthesis enables selective solar-to-chemical conversion by harnessing photoelectrocatalytic platforms to drive redox biocatalysis. However, the reliance of most photoelectrochemical (PEC)-based devices on transparent conductive oxides (TCOs) or wired configurations introduces resistive losses and architectural complexity, limiting the translation of biosolar conversion beyond laboratory-scale systems. Here, we report a wireless, monolithic semi-artificial leaf device toward scalable and practical solar biosynthesis. The PEC tandem, composed of a poly(ethylene glycol) (PEG)-modified BiVO4 (PEG:BiVO4) photoanode and a tunnel-oxide-passivated-contact (TOPCon) Si photovoltaic (PV), supplies sufficient photovoltage to reduce O2 to H2O2 on an anthraquinone-2-carboxylic acid (AQC)-functionalized carbon-fiber paper (CFP) cathode under solar light, sustaining over 100 h of stable operation. The photogenerated H2O2 reacts with peroxygenases to catalyze the oxyfunctionalization of substituted benzenes, alkanes, and fatty acids with record-high total turnover numbers of 166,100 (unspecific peroxygenase) and 3,700 (cytochrome P450). Furthermore, the scaling of the PEC device allows the direct conversion of natural light into enantiopure alcohols.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"27 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-10-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091724","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0