Energy & Environmental Materials最新文献

{"title":"Trifluorophenyl Side Chain Engineering in Benzotriazole-Core Acceptors for High-Performance Organic Photovoltaics","authors":"Sabeen Zahra,&nbsp;Du Hyeon Ryu,&nbsp;Jong-Woon Ha,&nbsp;Seungjin Lee,&nbsp;Muhammad Haris,&nbsp;Chang Eun Song,&nbsp;Hang Ken Lee,&nbsp;Sang Kyu Lee,&nbsp;Won Suk Shin","doi":"10.1002/eem2.12875","DOIUrl":"https://doi.org/10.1002/eem2.12875","url":null,"abstract":"<p>In this study, we explore an innovative approach to enhancing the photovoltaic performance of organic solar cells through core fluorination of the non-fullerene acceptor. We developed a benzotriazole-based non-fullerene acceptor with a trifluorinated phenyl side chain, referred to as YNPF3, which has a significant impact on the molecular properties, including a surprisingly varied local dipole moment and crystalline nature, as well as effectively stabilizing the frontier molecular orbital energy levels. Furthermore, a trifluoro-phenyl-based non-fullerene acceptor exhibits enhanced absorptivity, restricted voltage loss, and favorable photoactive morphology compared with its methyl side chain counterpart non-fullerene acceptor. Consequently, a binary organic solar cell based on YNPF3 achieves an outstanding power conversion efficiency of 19.2%, surpassing the control device with a efficiency of 16.5%. Finally, the YNPF3-based organic solar cell presents an impressive power conversion efficiency of 16.6% in a mini-module device with an aperture size of 12.5 cm², marking the highest reported efficiency for series-connected binary organic solar cells with a photoactive area over 10 cm².</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 3","pages":""},"PeriodicalIF":13.0,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12875","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836288","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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":"Poly(Norbornene-Diphenothiazine) for Electrochemical Capture and Release of Chromium and Arsenic Oxyanions from Water","authors":"Chen Li,&nbsp;Dandong Wang,&nbsp;Zhengyang Zhang,&nbsp;Jae Uk Choi,&nbsp;Jun Huang,&nbsp;Ki-Taek Bang,&nbsp;Shaopeng Xu,&nbsp;Yanming Wang,&nbsp;Yoonseob Kim","doi":"10.1002/eem2.12865","DOIUrl":"https://doi.org/10.1002/eem2.12865","url":null,"abstract":"<p>Drinking water contamination by heavy metals, particularly chromium and arsenic oxyanions, is a severe challenge threatening humanity's sustainable development. Electrochemically mediated water purification is gaining attention due to its high uptake, rapid kinetics, modularity, and facile regeneration. Here, we designed a composite electrode by combining a redox-active/Faradaic polymer, poly(norbornene-diphenothiazine) (PNP₂), with carbon nanotubes (CNTs) – PNP₂-CNT. The PNP₂-CNT demonstrated exceptional pseudocapacitance behavior, resulting in significantly accelerated adsorption rates for dichromate (Cr(VI); 0.008 g mg⁻¹ min⁻¹) and arsenite (As(III); 0.03 g mg⁻¹ min⁻¹), surpassing reported materials by a margin of 3–200 times, while demonstrating a high adsorption capacity, 666.3 and 612.4 mg g⁻¹, respectively. Furthermore, it effectively converted As(III) to the less toxic arsenate (As(V)) during adsorption and Cr(VI) to the less toxic chromium (Cr(III)) during desorption. This PNP₂-CNT system also showed significantly lower energy consumption, only 0.17% of the CNT control system. This study demonstrated for the first time the use of PNP₂ redox-active polymers in the separation and conversion process, meeting the six criteria of high uptake, rapid kinetics, selectivity, stability, recyclability, and energy efficiency. This achievement expands the scope of advanced materials that address environmental concerns and make an impact by generating energy- and cost-effective water purification.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 3","pages":""},"PeriodicalIF":13.0,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12865","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836117","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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":"Electrochemical Precipitation Energy-Assisted Aqueous Battery with High Voltage and High Electrode Utilization","authors":"Chang Liu,&nbsp;Lvzhang Jiang,&nbsp;Yu Liu","doi":"10.1002/eem2.12870","DOIUrl":"https://doi.org/10.1002/eem2.12870","url":null,"abstract":"<p>Increasing battery voltage and electrode utilization is of great significance for improving the energy density of aqueous battery. Herein, for the first time, this work introduces an integrated design strategy to regulate electrode potential and improve electrode utilization based on the concept of electrochemical precipitation energy. By coupling precipitation reaction with original electrode reaction, the Gibbs free energy change (<span></span><math>\u0000 <mrow>\u0000 <msub>\u0000 <mo>Δ</mo>\u0000 <mi>r</mi>\u0000 </msub>\u0000 <msup>\u0000 <mi>G</mi>\u0000 <mi>θ</mi>\u0000 </msup>\u0000 </mrow></math>) of the precipitation reaction is coupled to battery reaction's <span></span><math>\u0000 <mrow>\u0000 <msub>\u0000 <mo>Δ</mo>\u0000 <mi>r</mi>\u0000 </msub>\u0000 <msup>\u0000 <mi>G</mi>\u0000 <mi>θ</mi>\u0000 </msup>\u0000 </mrow></math>, thereby altering battery's voltage. Besides, the electrode reaction changes to solid-to-solid reaction after coupling with precipitation reaction, which can improve electrode utilization. The potential of Cu is reduced from 0.34 to −0.96 V (the lowest value among all the reported Cu anode) with a Cu utilization of 87.93% (without additional copper in electrolyte) by coupling Cu₂S's precipitation reaction. Furthermore, the potential of I₂ is increased from 0.54 to 0.65 V (I₂/CuI) and 0.73 V (I₂/PbI₂) by coupling precipitation reaction of CuI and PbI₂ and the shutting effect of I₃⁻ is also limited. As proof of concept, a full Cu₂S battery (cathode: S/Cu₂S, anode: Cu/Cu₂S) is designed with average discharge voltage of 1.12 V, which is the highest value among all the Cu-based aqueous batteries. Due to the certain universality of this strategy, this work provides a new path to regulate the electrode reaction potential and improve electrode utilization.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 3","pages":""},"PeriodicalIF":13.0,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12870","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836118","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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":"Electrospun Carbon Nanofibers with Numerous Miniature Carbon Nanofibers for Free-Standing, Binder/Conductive Additive-Free Lithium-Ion Battery Anodes","authors":"Sehwa Hong,&nbsp;Siwan Kim,&nbsp;Minsun Kim,&nbsp;Songeui Bae,&nbsp;Hyeonsu Yang,&nbsp;Seulgee Lee,&nbsp;Yongsup Yun,&nbsp;Hyemin Kim,&nbsp;Daewook Kim,&nbsp;Jun Kang","doi":"10.1002/eem2.12874","DOIUrl":"https://doi.org/10.1002/eem2.12874","url":null,"abstract":"<p>Among their several unique properties, the high electrical conductivity and mechanical strength of carbon nanofibers make them suitable for applications such as catalyst support for fuel cells, flexible electrode materials for secondary batteries, and sensors. However, their performance requires improvement for practical applications. Several methods have been pursued to achieve this, such as growing carbon nanotubes from carbon nanofibers; however, the transition metal catalyst used to grow carbon nanotubes causes problems, including side reactions. This study attempts to address this issue by growing numerous branched carbon nanofibers from the main carbon nanofibers using alkali metals. Excellent electrical conductivity is achieved by growing densely branched carbon nanofibers. Consequently, a current collector, binder, and conductive material-free anode material is realized, exhibiting excellent electrochemical performance compared with existing carbon nanofibers. The proposed method is expected to be a powerful tool for secondary batteries and have broad applicability to various fields.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 3","pages":""},"PeriodicalIF":13.0,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12874","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143835795","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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":"Highly Ion-Conductive 3D Hybrid Solid Polymer Electrolyte Using Al-Doped Li7La3Zr2O12 Embedded Electrospun 3D Nanowebs for Ambient-Temperature All-Solid Lithium Polymer Batteries","authors":"Getachew Mengesha Biressaw,&nbsp;Tien Manh Nguyen,&nbsp;Do Youb Kim,&nbsp;Dong Wook Kim,&nbsp;Jungdon Suk,&nbsp;Yongku Kang","doi":"10.1002/eem2.12860","DOIUrl":"https://doi.org/10.1002/eem2.12860","url":null,"abstract":"<p>Solid polymer electrolytes have garnered significant attention for lithium batteries because of their flexibility and safety. However, poor ionic conductivity, lithium dendrite formation, and high impedance hinder their practical application. In this study, a thin, flexible, 3D hybrid solid electrolyte (3DHSE) is prepared by in situ thermal cross-linking polymerization with electrospun 3D nanowebs. The 3DHSE comprises Al-doped Li₇La₃Zr₂O₁₂ (ALLZO) embedded in electrospun poly(vinylidene fluoride-<i>co</i>-hexafluoropropylene) (PVDF-HFP) nonwoven 3D nanowebs and an in situ cross-linked polyethylene oxide (PEO)-based solid polymer electrolyte. The 3DHSE exhibits high tensile strength (6.55 MPa), a strain of 40.28%, enhanced ionic conductivity (7.86 × 10⁻⁴ S cm⁻¹), and a superior lithium-ion transference number (0.76) to that of the PVDF-HFP-based solid polymer electrolyte (PSPE). This enables highly stable lithium plating/stripping cycling for over 900 h at 25 °C with a current density of 0.2 mA cm⁻². The LiNi_0.8Mn_0.1Co_0.1O₂ (NCM811)/3DHSE/Li cell has a higher capacity (140.56 mAh g⁻¹ at 0.1 C) than the NCM811/PSPE/Li cell (124.88 mAh g⁻¹ at 0.1 C) at 25 °C. The 3DHSE enhances mechanical properties, stabilizes interfacial contact, improves ion transport, prevents NCM811 cracking, and significantly boosts cycling performance. This study highlights the potential of the 3DHSE as a candidate for advanced lithium polymer battery technology.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 3","pages":""},"PeriodicalIF":13.0,"publicationDate":"2025-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12860","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143835980","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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":"Unveiling the Potential of Metal Diborides for Electrocatalytic Water Splitting: A Comprehensive Review","authors":"Ebrahim Sadeghi,&nbsp;Sanaz Chamani,&nbsp;Naeimeh Sadat Peighambardoust,&nbsp;Umut Aydemir","doi":"10.1002/eem2.12873","DOIUrl":"https://doi.org/10.1002/eem2.12873","url":null,"abstract":"<p>Electrocatalytic water splitting (EWS) driven by renewable energy is vital for clean hydrogen (H₂) production and reducing reliance on fossil fuels. While IrO₂ and RuO₂ are the leading electrocatalysts for the oxygen evolution reaction (OER) and Pt for the hydrogen evolution reaction (HER) in acidic environments, the need for efficient, stable, and affordable materials persists. Recently, transition-metal borides (TMBs), particularly metal diborides (MDbs), have gained attention due to their unique layered crystal structures with multicentered boron bonds, offering remarkable physicochemical properties. Their nearly 2D structures boost electrochemical performance by offering high conductivity and a large active surface area, making them well-suited for advanced energy storage and conversion technologies. This review provides a comprehensive overview of the critical factors for water splitting, the crystal and electronic structures of MDbs, and their synthetic strategies. Furthermore, it examines the relationship between catalytic performance and intermediate adsorption as elucidated by first-principle calculations. The review also highlights the latest experimental advancements in MDb-based electrocatalysts and addresses the current challenges and future directions for their development.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 3","pages":""},"PeriodicalIF":13.0,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12873","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836165","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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":"In Situ Formation of Bifunctional Interlayer on 3D Conductive Scaffold for Dendrite-Free Li Metal Batteries","authors":"Yonghwan Kim,&nbsp;Dohyeong Kim,&nbsp;Minjun Bae,&nbsp;Yujin Chang,&nbsp;Won Young An,&nbsp;Hwichan Hong,&nbsp;Seon Jae Hwang,&nbsp;Dongwan Kim,&nbsp;Jeongyeon Lee,&nbsp;Yuanzhe Piao","doi":"10.1002/eem2.12861","DOIUrl":"https://doi.org/10.1002/eem2.12861","url":null,"abstract":"<p>Regulating lithium (Li) plating/stripping behavior in three-dimensional (3D) conductive scaffolds is critical to stabilizing Li metal batteries (LMBs). Surface protrusions and roughness in these scaffolds can induce uneven distributions of the electric fields and ionic concentrations, forming “hot spots.” Hot spots may cause uncontrollable Li dendrites growth, presenting significant challenges to the cycle stability and safety of LMBs. To address these issues, we construct a Li ionic conductive-dielectric gradient bifunctional interlayer (ICDL) onto a 3D Li-injected graphene/carbon nanotube scaffold (LGCF) via in situ reaction of exfoliated hexagonal boron nitride (fhBN) and molten Li. Microscopic and spectroscopic analyses reveal that ICDL consists of fhBN-rich outer layer and inner layer enriched with Li₃N and Li-boron composites (Li-B). The outer layer utilizes dielectric properties to effectively homogenize the electric field, while the inner layer ensures high Li ion conductivity. Moreover, DFT calculations indicate that ICDL can effectively adsorb Li and decrease the Li diffusion barrier, promoting enhanced Li ion transport. The modulation of Li kinetics by ICDL increases the critical length of the Li nucleus, enabling suppression of Li dendrite growth. Attributing to these advantages, the ICDL-coated LGCF (ICDL@LGCF) demonstrates impressive long-term cycle performances in both symmetric cells and full cells.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 3","pages":""},"PeriodicalIF":13.0,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12861","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836166","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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":"Enhancing Alkaline Hydrogen Evolution Reaction on Ru-Decorated TiO2 Nanotube Layers: Synergistic Role of Ti3+, Ru Single Atoms, and Ru Nanoparticles","authors":"Sitaramanjaneya Mouli Thalluri,&nbsp;Jhonatan Rodriguez-Pereira,&nbsp;Jan Michalicka,&nbsp;Eva Kolíbalová,&nbsp;Ludek Hromadko,&nbsp;Stanislav Slang,&nbsp;Miloslav Pouzar,&nbsp;Hanna Sopha,&nbsp;Raul Zazpe,&nbsp;Jan M. Macak","doi":"10.1002/eem2.12864","DOIUrl":"https://doi.org/10.1002/eem2.12864","url":null,"abstract":"<p>Synergistic interplays involving multiple active centers originating from TiO₂ nanotube layers (TNT) and ruthenium (Ru) species comprising of both single atoms (SAs) and nanoparticles (NPs) augment the alkaline hydrogen evolution reaction (HER) by enhancing Volmer kinetics from rapid water dissociation and improving Tafel kinetics from efficient H* desorption. Atomic layer deposition of Ru with 50 process cycles results in a mixture of Ru SAs and 2.8 ± 0.4 nm NPs present on TNT layers, and it emerges with the highest HER activity among all the electrodes synthesized. A detailed study of the Ti and Ru species using different high-resolution techniques confirmed the presence of Ti³⁺ states and the coexistence of Ru SAs and NPs. With insights from literature, the role of Ti³⁺, appropriate work functions of TNT layers and Ru, and the synergistic effect of Ru SAs and Ru NPs in improving the performance of alkaline HER were elaborated and justified. The aforementioned characteristics led to a remarkable performance by having 9 mV onset potentials and 33 mV dec⁻¹ of Tafel slopes and a higher turnover frequency of 1.72 H₂ s⁻¹ at 30 mV. Besides, a notable stability from 28 h staircase chronopotentiometric measurements for TNT@Ru surpasses TNT@Pt in comparison.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 3","pages":""},"PeriodicalIF":13.0,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12864","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143835840","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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":"Approaching Theoretical Limit of Ta3N5 Photoanode via Photothermal-Accelerating Kinetics with Full-Spectrum Utilization","authors":"Yi Liu,&nbsp;Yanwei Zhang,&nbsp;Yi-Cheng Wang,&nbsp;Xiaopeng Zhan,&nbsp;Peng-Fei Sui,&nbsp;Jing-Li Luo,&nbsp;Chenyu Xu","doi":"10.1002/eem2.12868","DOIUrl":"https://doi.org/10.1002/eem2.12868","url":null,"abstract":"<p>Tantalum nitride is widely considered as a promising photoanode material for its suitable band structure as well as the high theoretical conversion efficiency in solar water splitting. However, it is limited to inefficient photoinduced electron–hole pair separation and interfacial dynamics in the photoelectrochemical oxygen evolution reaction. Herein, multiple layers including Ti_<i>x</i>Si_<i>y</i> and NiFeCoO_<i>x</i> were fabricated based on band engineering to regulate tandem electric states for efficient transfer of energy carriers. Besides, photothermal local surface plasmon resonance was introduced to accelerate the kinetics of photoelectrochemical reactions at the interface when the special Ag nanoparticles were loaded to extend the absorbance to near infrared light. Consequently, a recordable photocurrent density of 12.73 mA cm⁻² has been achieved at 1.23 V versus RHE, approaching a theoretical limit of the tantalum nitride photoanode with full-spectrum solar utilization. Meanwhile, compared to the applied bias photon-to-current efficiency of 1.36% without photothermal factor, a high applied bias photon-to-current efficiency of 2.27% could be raised by applying local surface plasmon resonance to photoelectrochemical oxygen evolution reaction. The efficient design could maximize the use of solar light via the classification of spectrum and, therefore, may spark more innovative ideas for the future design and development of the next-generation photoelectrode.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 3","pages":""},"PeriodicalIF":13.0,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12868","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836213","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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":"An Efficient Thick Electrode Design with Artificial Porous Structure and Gradient Particle Arrangement for Lithium-Ion Batteries","authors":"Zhichen Du,&nbsp;Quanbin Zha,&nbsp;Zihan Zhang,&nbsp;Qin Chen,&nbsp;Hui Yang,&nbsp;Zhouguang Lu,&nbsp;Tianyou Zhai,&nbsp;Huiqiao Li","doi":"10.1002/eem2.12867","DOIUrl":"https://doi.org/10.1002/eem2.12867","url":null,"abstract":"<p>Thick electrode, with its feasibility and cost-effectiveness in lithium-ion batteries (LIBs), has attracted significant attention as a promising approach maximizing the energy density of battery. Through raising the mass loading of active materials without altering the fundamental chemical attributes, thick electrodes can boost the energy density of the batteries effectively. Nevertheless, as the thickness of the electrode increases, the ionic conductivity of the electrode decreases, leading to abominable polarization in the thickness direction, which severely hampers the practical application of a thick electrode. This work proposes a novel porous gradient design of high-performance thick electrodes for LIBs. By constructing a porous structure that serves as a fast transport pathway for lithium (Li) ions, the ion transport kinetics within thick electrodes are significantly enhanced. Meanwhile, a particle size gradient design is incorporated to further mitigate polarization effects within the electrode, leading to substantial improvements in reaction homogeneity and material utilization. Employing this strategy, we have fabricated a porous gradient nanocellulose-carbon-nanotube based thick electrode, which exhibits an impressive capacity retention of 86.7% at a high mass loading of LiCoO₂ (LCO) active material (20 mg cm⁻²) and a high current density of 5 mA cm⁻².</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 3","pages":""},"PeriodicalIF":13.0,"publicationDate":"2025-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12867","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836212","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}