CarbonPub Date : 2025-07-21DOI: 10.1016/j.carbon.2025.120648
Zhaojin Li , Zezhao Li , Chenze Di , Di Zhang , Qiujun Wang , Huilan Sun , Qujiang Sun , Fei Yuan , Ranran Li , Bo Wang
{"title":"Mechanistic insights into oxygen–boron co-doping in activated carbon: Tailoring surface chemistry and wettability","authors":"Zhaojin Li , Zezhao Li , Chenze Di , Di Zhang , Qiujun Wang , Huilan Sun , Qujiang Sun , Fei Yuan , Ranran Li , Bo Wang","doi":"10.1016/j.carbon.2025.120648","DOIUrl":"10.1016/j.carbon.2025.120648","url":null,"abstract":"<div><div>Oxygen (O) and Boron (B) heteroatom doping has emerged as a promising strategy to enhance the capacitive performance of activated carbon (AC) for supercapacitors. However, the synergistic mechanism between these heteroatoms remains ambiguous due to intertwined morphological and compositional changes during conventional doping processes. This study employs a stepwise doping methodology to independently control O and B concentrations while preserving the structural integrity of AC. Through sequential high-temperature B doping and low-temperature oxidation, dual-doped AC (AC-<em>O</em>-B) retains comparable specific surface area and pore structure to pristine AC. Electrochemical evaluations reveal that O–B double doping has no significant effect on the double-layer capacitance, but it greatly improves the pseudocapacitance. Mechanistic analysis demonstrates that O doping introduces abundant C–O groups and facilitating the formation of BC<sub>2</sub>O structures via B integration. The presence of C–O groups and BC<sub>2</sub>O structure not only enhance surface wettability but also optimize charge transfer kinetics and redox-active site density. This work provides critical insights into heteroatom co-doping strategies for designing high-performance carbon-based supercapacitors.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"244 ","pages":"Article 120648"},"PeriodicalIF":10.5,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144711325","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
CarbonPub Date : 2025-07-21DOI: 10.1016/j.carbon.2025.120644
Yingxian Wang , Ning Sun , Bin Qiu , Weijie Chen , Weiwei Pang , Bin Xu
{"title":"Defect-functionality synergistic strategy enabling uniform Na plating for dendrite-free sodium metal anodes","authors":"Yingxian Wang , Ning Sun , Bin Qiu , Weijie Chen , Weiwei Pang , Bin Xu","doi":"10.1016/j.carbon.2025.120644","DOIUrl":"10.1016/j.carbon.2025.120644","url":null,"abstract":"<div><div>Sodium metal batteries (SMBs) are promising candidates for next-generation high-energy batteries due to the abundance and low cost of sodium. However, their practical deployment is hindered by uneven sodium deposition and dendritic growth, which leads to poor cycling stability and safety concerns. Herein, sodiophilic porous carbon hosts are fabricated via a defect engineering and surface functionalization strategy. The incorporation of moderate structural defects effectively reduces the sodium nucleation overpotential, while the oxygen-containing functional groups such as carboxyl (–COOH) and carbonyl (C=O) guides the formation of dense and uniform sodium layers. Theoretical calculations and experimental characterizations collectively reveal the synergistic role of defect sites and surface functionalities in promoting Na<sup>+</sup> diffusion and regulating nucleation behavior. Consequently, the optimized ABC-11 achieves exceptional cycling stability with a Coulombic efficiency of 99.91 % over 1200 cycles at 1 mA cm<sup>−2</sup>/1 mAh cm<sup>−2</sup> in asymmetric cells. The Na@ABC-11 symmetric cell also exhibits ultra-stable plating/stripping durability exceeding 2200 h. Furthermore, the assembled Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> || Na@ABC-11 full cell delivers a high reversible capacity of 102 mAh g<sup>−1</sup> and maintains 94 % of its initial capacity after 1200 cycles. This work highlights a cost-effective and scalable strategy for the structural design of carbon-based hosts, offering a viable pathway toward high-performance SMBs.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"244 ","pages":"Article 120644"},"PeriodicalIF":10.5,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144702670","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
CarbonPub Date : 2025-07-21DOI: 10.1016/j.carbon.2025.120647
Jian Wang , Ying Shi , Chengxu Rong , Yulin Li , Zhuyin Sui , Xiufeng Xu
{"title":"Self-activated microporous carbon with tailored pore structures and surface polarity for efficient SF6/N2 and NF3/N2 separation","authors":"Jian Wang , Ying Shi , Chengxu Rong , Yulin Li , Zhuyin Sui , Xiufeng Xu","doi":"10.1016/j.carbon.2025.120647","DOIUrl":"10.1016/j.carbon.2025.120647","url":null,"abstract":"<div><div>Adsorption-based separation of SF<sub>6</sub> and NF<sub>3</sub> from N<sub>2</sub> represents a promising strategy for resource recovery and environmental mitigation. However, the development of cost-effective adsorbents possessing precisely engineered structures for high efficiency remains challenging. This study introduces a straightforward, self-activation method for synthesizing microporous carbon adsorbents through the direct pyrolysis of polyvinylidene fluoride (PVDF) resin. This approach enables the simultaneous tailoring of micropore size distribution for size matching and the in-situ surface polarity modulation via polar oxygen and residual fluorine functional groups. By adjusting pyrolysis temperatures from 600 to 900 °C, we obtained an optimal PVDF-800 with a high concentration of micropores centered at ∼0.68 nm. The combination of tuned pore structure and enhanced polarity results in competitive static adsorption capacities for SF<sub>6</sub> (1.93 mmol g<sup>−1</sup>) and NF<sub>3</sub> (0.57 mmol g<sup>−1</sup>) at 298 K and 0.1 bar, coupled with moderate adsorption affinities for regeneration. Dynamic breakthrough experiments under binary mixtures confirm the effective separation performance and cyclic stability of PVDF-800. Critically, PVDF-800 demonstrates efficient desorption performance at 298 K, yielding 1.17 mmol g<sup>−1</sup> SF<sub>6</sub> and 0.13 mmol g<sup>−1</sup> NF<sub>3</sub> with ≥99.9 % purity. These results highlight the significance of concurrently optimizing pore size and surface polarity for developing high-performance porous adsorbents for F-gas separation.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"244 ","pages":"Article 120647"},"PeriodicalIF":10.5,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144702672","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
CarbonPub Date : 2025-07-19DOI: 10.1016/j.carbon.2025.120613
Mustafa K. Bayazit , Hin Chun Yau , Christopher S. Roberts , Joachim H.G. Steinke , Milo S.P. Shaffer
{"title":"A diameter selective fullerene-mediated supramolecular self-assembly motif for single-walled carbon nanotube enrichment","authors":"Mustafa K. Bayazit , Hin Chun Yau , Christopher S. Roberts , Joachim H.G. Steinke , Milo S.P. Shaffer","doi":"10.1016/j.carbon.2025.120613","DOIUrl":"10.1016/j.carbon.2025.120613","url":null,"abstract":"<div><div>Post-synthetic diameter-selective separation of nanotubular structures has relied on exohedral interactions; a diameter-dependent enrichment via endohedral interactions for the purification of bulk single-walled carbon nanotubes (SWCNTs) remains unexplored. This paper describes a novel diameter-selective supramolecular self-assembly motif for nanotube enrichment via fullerene (C<sub>60</sub>) encapsulation by SWCNTs. C<sub>60</sub>-grafted silicon wafers and silica particles were used for the diameter-selective self-assembly and enrichment/separation of individualized SWCNTs, respectively. C<sub>60</sub> grafting to silica substrates was performed via the addition of azide-terminated silane precursors, followed by the cycloaddition of azides with C<sub>60</sub> to azafulleroids. Atomic force microscopy was used to determine the diameter dependency of the method. The diameter-sorted SWCNTs were further characterized via ultraviolet–visible–near-infrared spectroscopy and Raman spectroscopy. The method presented here was found to select SWCNTs with diameters of approximately 1.4–1.7 nm, with a central cavity matched to the diameter of C<sub>60</sub>. Self-assembly and enrichment/separation of other nanotubular structures are anticipated with this approach.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"244 ","pages":"Article 120613"},"PeriodicalIF":10.5,"publicationDate":"2025-07-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144702671","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
CarbonPub Date : 2025-07-19DOI: 10.1016/j.carbon.2025.120639
Yanqing Cong , Yijun Mo , Jiahong Pan , Xinyi Shen , Chenyi Wang , Ziyi Guo , Liwen Fan , Xinyue Li , Shi-Wen Lv
{"title":"Regulating exciton generation and transfer upon nanoarchitectonics with carbon nitrogen polymer for photocatalytic hydrogen peroxide evolution coupled with ethanol selective oxidation","authors":"Yanqing Cong , Yijun Mo , Jiahong Pan , Xinyi Shen , Chenyi Wang , Ziyi Guo , Liwen Fan , Xinyue Li , Shi-Wen Lv","doi":"10.1016/j.carbon.2025.120639","DOIUrl":"10.1016/j.carbon.2025.120639","url":null,"abstract":"<div><div>Efficient generation and rapid transfer of photogenerated carriers are crucial for the improvement of photocatalytic reaction. Herein, pyromellitic anhydride as electron acceptor is embedded into porous g-C<sub>3</sub>N<sub>4</sub> for constructing D-A polymer (namely P-g–C<sub>3</sub>N<sub>4</sub>–Pa). The introduction of pyromellitic anhydride effectively improves π→π∗ and n→π∗ electronic transitions, enhancing light utilization efficiency. Significant potential difference between pyromellitic anhydride and g-C<sub>3</sub>N<sub>4</sub> weakens excitonic effect to produce free electrons and holes. Thus, P-g–C<sub>3</sub>N<sub>4</sub>–Pa exhibits excellent performance in photocatalytic H<sub>2</sub>O<sub>2</sub> synthesis. In-situ spectroscopy and electrochemical tests reveal that two-electron oxygen reduction reaction is major pathway, and O<sub>2</sub><sup>•‒</sup> is a key intermediate. Embedded pyromellitic anhydride also boosts capture capability of g-C<sub>3</sub>N<sub>4</sub> for O<sub>2</sub>, thereby overcoming rate-limiting step to promote ∗O<sub>2</sub> generation. Furthermore, photogenerated holes located on g-C<sub>3</sub>N<sub>4</sub> can selectively oxidize ethanol to produce acetaldehyde with high economic value, and generated proton facilitates H<sub>2</sub>O<sub>2</sub> generation. Importantly, the highest yield of H<sub>2</sub>O<sub>2</sub> is 5600.8 μmol g<sup>−1</sup>•h<sup>−1</sup> over P-g–C<sub>3</sub>N<sub>4</sub>–Pa under visible light irradiation in the presence of ethanol.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"244 ","pages":"Article 120639"},"PeriodicalIF":10.5,"publicationDate":"2025-07-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144662327","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
CarbonPub Date : 2025-07-19DOI: 10.1016/j.carbon.2025.120641
Huan Li , Minghui Zhao , Yun Wu , Xiaomin Yang , Zihan Yang , Le Chen , Jingtai Zhao , Wentao Zhang , Jinliang Li
{"title":"Step-temperature strategy enables closed-pores in hard carbon achieving high plateau capacity for sodium ion storage","authors":"Huan Li , Minghui Zhao , Yun Wu , Xiaomin Yang , Zihan Yang , Le Chen , Jingtai Zhao , Wentao Zhang , Jinliang Li","doi":"10.1016/j.carbon.2025.120641","DOIUrl":"10.1016/j.carbon.2025.120641","url":null,"abstract":"<div><div>Hard carbon (HC) has become the most promising anode material for sodium ion batteries (SIBs) due to its high reversible capacity, adjustable conductivity and low platform potential. However, the presence of numerous defects often results in relatively low capacity in the low-voltage plateau region (<0.1 V) and poor initial Coulombic efficiency (ICE). Closed pores in HC are widely regarded as a critical factor for enhancing plateau capacity. In this study, we utilized step-temperature strategy to stabilize the oxygen-centered radicals in biomass, which in turn mediated the topological reconstruction process of carbon microcrystals. This strategy increases the closed porosity of HC by accurately adjusting the curvature of the carbon layer, promotes the orderly reorganization of the carbon layer, and inhibits the problem of low closed porosity caused by excessive structural crosslinking. On this basis, the optimized HC has a high specific capacity of 339 mAh g<sup>−1</sup> at 100 mA g<sup>−1</sup>, and has an ultra-high capacity retention rate of 97.5 % after 100 cycles. The platform capacity is increased from 142 mAh g<sup>−1</sup> to 232 mAh g<sup>−1</sup>, and ICE is increased to 80.1 %. Furthermore, the electrochemical mechanism of sodium storage under pore structure regulation was investigated using in situ Raman spectroscopy, elucidating the electrochemical reactions during different sodiation-desodiation processes.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"244 ","pages":"Article 120641"},"PeriodicalIF":10.5,"publicationDate":"2025-07-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144694517","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
CarbonPub Date : 2025-07-19DOI: 10.1016/j.carbon.2025.120642
Jason Thamizhakaran Stanley , Pragati A. Shinde , Renzhi Ma , Jonathan P. Hill , Katsuhiko Ariga , Sivanesan Subramanian , Lok Kumar Shrestha
{"title":"Nanoarchitectonic grafting of NiCo-layered double hydroxide on fullerene-derived carbon nanorods for hybrid supercapacitors","authors":"Jason Thamizhakaran Stanley , Pragati A. Shinde , Renzhi Ma , Jonathan P. Hill , Katsuhiko Ariga , Sivanesan Subramanian , Lok Kumar Shrestha","doi":"10.1016/j.carbon.2025.120642","DOIUrl":"10.1016/j.carbon.2025.120642","url":null,"abstract":"<div><div>Improving the electrochemical performance of hybrid supercapacitors (HSCs) through the synergistic modulation of battery-type materials with nanoporous carbon is a crucial strategy for advancing energy storage. In this study, we synthesized NiCo-layered double hydroxides on fullerene-derived carbon nanorods (FNR-800@NiCo-LDH) via high-temperature carbonization of fullerene nanorods followed by a hydrothermal process. The encapsulation of NiCo-LDH on FNR-800 results in excellent electrochemical performance due to the multi-oxidation states of nickel and cobalt species and the high surface area of FNR-800. The FNR-800@NiCo-LDH electrode exhibits battery-type redox behavior with a high specific capacitance of 1396.1 F g<sup>−1</sup> at 1 A g<sup>−1</sup>, a good rate capability of 69.8 %, and superior cycling stability of 93.1 % over 5000 cycles. Additionally, an asymmetric cell constructed with FNR-800@NiCo-LDH as the positive electrode and FNR-800 carbon as the negative electrode demonstrated a specific energy of 68.8 Wh kg<sup>−1</sup> at a specific power of 800 W kg<sup>−1</sup>, along with high rate capability and excellent cycle stability over 5000 cycles. This strategy of integrating metallic species with carbon nanoarchitecture effectively regulates the redox activity of materials, paving the way for their practical application in future energy storage applications.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"244 ","pages":"Article 120642"},"PeriodicalIF":10.5,"publicationDate":"2025-07-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144714203","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
CarbonPub Date : 2025-07-18DOI: 10.1016/j.carbon.2025.120638
Qian Xu , Lu Guo , Huiyu Yu , Yongheng Zhang , Ting Liu , Junwei Han , Linjie Zhi
{"title":"Electronegative interface modification enables accelerated interfacial kinetics for lithium-ion battery anodes","authors":"Qian Xu , Lu Guo , Huiyu Yu , Yongheng Zhang , Ting Liu , Junwei Han , Linjie Zhi","doi":"10.1016/j.carbon.2025.120638","DOIUrl":"10.1016/j.carbon.2025.120638","url":null,"abstract":"<div><div>The mainstream graphite anode in lithium batteries encounters obstacles including the capacity reduction and polarization during fast-charging, which is mainly restricted by the sluggish ion transfer kinetics. Here, a universal electronegative interfacial modification strategy is proposed for improving the fast-charging performance of the graphite (Gr) anode, in which the electronegative –COOH groups on the graphite/electrolyte interface serve as a Li<sup>+</sup> reservoir by the pre-adsorption of a large amount of Li<sup>+</sup> through electrostatic interaction. The electron-rich interface and the enrichment of Li<sup>+</sup> at the interface weaken the Li<sup>+</sup>-solvent interaction and provide a larger Li<sup>+</sup> potential difference, thereby accelerating desolvation process and inducing the formation of inorganic-rich SEI. Therefore, the interfacial kinetics of the graphite anode was enhanced substantially by the weakened Li<sup>+</sup>-solvent interaction and LiF-rich SEI interface. As a result, the Gr@rGO anode with optimized –COOH groups and appropriate defects achieved a great rate performance of 192 mAh g<sup>−1</sup> at 4C, small polarization of 0.026 V, and excellent cycling stability with 97 % after 600 cycles in pouch cells. In addition, universal application of –COOH modified interphase for fast-charging performance in high-energy-density anode systems, including SiO and nano-silicon anodes, was proved to be feasible, revealing the effectiveness of the electronegative regulation for fast-charging lithium-ion battery anodes.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"244 ","pages":"Article 120638"},"PeriodicalIF":10.5,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144694516","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
CarbonPub Date : 2025-07-17DOI: 10.1016/j.carbon.2025.120636
Guidong Chi , Zixuan Dai , Xinyi Liu , Zhenming Li , Wei Liu , Maolin Li , Zhonghao Wang , Lingxiao Cao , Xiangfei Wang , Daiwei Hu , Dehai Yu , Shun Ma , Xindong Ni , Zhen Li , Zhizhu He , Quan Zhou
{"title":"Multilayer dual-embedded temperature-pressure synergized sensing of “breathing effect” in lithium-ion cells","authors":"Guidong Chi , Zixuan Dai , Xinyi Liu , Zhenming Li , Wei Liu , Maolin Li , Zhonghao Wang , Lingxiao Cao , Xiangfei Wang , Daiwei Hu , Dehai Yu , Shun Ma , Xindong Ni , Zhen Li , Zhizhu He , Quan Zhou","doi":"10.1016/j.carbon.2025.120636","DOIUrl":"10.1016/j.carbon.2025.120636","url":null,"abstract":"<div><div>The “breathing effect,” as an inherent phenomenon exhibited by lithium-ion batteries (LIBs) during operation, can serve as a significant basis for identifying the battery's State of Charge (SOC) and State of Health (SOH). However, the existing single-parameter sensor is insufficient to elucidate the operating mechanism owing to the complex behavior of batteries. Herein, a high-performance carbon-based temperature-pressure thin-film (CTPF) sensor is fabricated based on carbon nanotube (CNT)/laser-induced graphene (LIG)/LIG-styrene ethylene butylene styrene (SEBS). The CTPF shows a wide sensing range (≤768 kPa for pressure, −20∼120 °C for temperature), fast pressure response (83 ms) and recovery (156 ms) speed, and good stability (above 5000 pressure cycles, above 2200 min temperature stage-cycles) with only 143 μm thickness. In addition, the CTPF shows good temperature-pressure decoupling performance attributable to its unique multilayer dual-embedded structure. By taking advantage of a cell sensing system (CSS), the “breathing effect” of a single cell is monitored and corresponds with the phase transition stages. A relationship between the module's SOC, C-rate, pressure and temperature is identified, and an anomaly phenomenon “gas evolution-redissolution” in the module is observed, which offers an additional method to monitor the SOC and SOH. Some extreme conditions are also studied for early damage warning. This work offers valuable insights and the foundation for future applications in wearable monitoring of lithium-ion batteries.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"244 ","pages":"Article 120636"},"PeriodicalIF":10.5,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144653863","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
CarbonPub Date : 2025-07-17DOI: 10.1016/j.carbon.2025.120637
Hongdian Chen , Chenyang Shu , Jianglin Chen , Jinyan Wu , Rong Jin , Yao Liu , Chuanlan Xu , Chaozhong Guo , Yujun Si
{"title":"Zinc-mediated activator crafting of single-atomic Mn–N2|Zn–N6 sites and nanoclusters within microporous carbon networks for efficient oxygen reduction","authors":"Hongdian Chen , Chenyang Shu , Jianglin Chen , Jinyan Wu , Rong Jin , Yao Liu , Chuanlan Xu , Chaozhong Guo , Yujun Si","doi":"10.1016/j.carbon.2025.120637","DOIUrl":"10.1016/j.carbon.2025.120637","url":null,"abstract":"<div><div>Metal-organic frameworks (MOFs) serve as superior precursors for porous carbon electrocatalysts due to tailorable coordination environments and structural adaptability. However, pyrolysis-induced structural degradation causes metallic aggregation and pore disorder, severely impairing oxygen reduction reaction (ORR) kinetics. We develop a confined ZnCl<sub>2</sub> etching strategy to convert metal triazolate frameworks into microporous-dominated ZnMn–N–C catalysts, exposing active sites at triple-phase interfaces. Molten ZnCl<sub>2</sub> simultaneously engineers microporores and suppresses metal coalescence, yielding atomically dispersed Mn–N<sub>2</sub>|Zn–N<sub>6</sub> moieties. The optimized catalyst achieves a 0.867 V half-wave potential (vs. RHE) in an alkaline media. In zinc-air batteries, it delivers 889 mWh g<sup>−1</sup><sub>Zn</sub> at 50 mA cm<sup>−2</sup> with 49 mV day over 150 h, while maintaining a <0.87 V charge-discharge gap at 10 mA cm<sup>−2</sup> for over 100 h. This work provides a rational strategy for spatially optimizing active sites via confined chemical etching, demonstrating significant potential for developing durable zinc-air batteries with enhanced reaction kinetics.</div></div>","PeriodicalId":262,"journal":{"name":"Carbon","volume":"244 ","pages":"Article 120637"},"PeriodicalIF":10.5,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144653859","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}