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JOURNAL OF SOLID STATE ELECTROCHEMISTRY · 2023 ·Vol. 27 ·期 5 ·1165-1175 · IF 2.5

A high-performance binder-free freestanding film anode constructed by Si/NC nanoparticles anchoring in 3D porous N-doped graphene-CNTs networks for Li-ion batteries

Liu Shuling,Zhang Wei,An Yiming,Li Ying,Wang Jie,Wang Chao

The Si-based flexible electrodes attracted increasing research interests owing to the growing demand for high-performance flexible energy storage devices. Herein, a facile and smart self-assembly strategy is adopted to address huge volume expansion and particle aggregation issues of Si-based anodes, and a high-performance freestanding film anode (NC@Si/CNTs/N-rGO) is synthesized. The 3D-crosslinked porous graphene-CNTs networks offer abundant electric conductive pathways, high active sites, large internal space to accommodate the expansion of Si NPs, and facilitate Li + diffusion and insertion/extraction kinetics. The synergistic effect between the well-dispersed Si/NC nanoparticles and 3D porous networks significantly enhances electrochemical performance of Si NPs. The as-prepared NC@Si/CNTs/N-rGO electrode exhibits a high reversible specific capacity of 1089 mAh·g −1 at a charge–discharge current density of 1 A·g −1 after 500 cycles. Even at 2 A·g −1 , the electrode still exhibits an excellent reversible specific capacity of 606 mAh·g −1 after 300 cycles. These indicate that the NC@Si/CNTs/N-rGO is a promising candidate for high-performance flexible anode material in lithium-ion batteries.

研究领域: 材料科学 · 电化学 · 纳米科技 · 能源存储 · 先进电池技术
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ELECTROCHIMICA ACTA · 2019 · IF 5.383

V2(PO4)O encapsulated into crumpled nitrogen-doped graphene as a high-performance anode material for sodium-ion batteries

Bin Xiao,Wen-hai Zhang,Peng-bo Wang,Lin-bo Tang,Chang-sheng An,Zhen-jiang He,Hui Tong,Jun-chao Zheng,Bo Wang

Phosphate-based polyanion-structured materials have attracted considerable attention as anode materials in lithium-/sodium-ion batteries due to their stable crystal structure, affordability, and environmental friendliness. V 2 (PO 4 )O was encapsulated into crumpled nitrogen-doped graphene (VPO@N-G) through a facile spray-drying method in which VPO particles were completely encapsulated by N-doped graphene. For the first time, VPO@N-G was explored as an anode material for sodium-ion batteries. The Na + storage behavior of VPO@N-G was systematically investigated at the voltage range of 0.01–3.0 V (versus Na/Na + ). Results indicated that the VPO@N-G anode can deliver a highly reversible discharge capacity of 539 mAh g −1  at 0.05 A g −1 and achieve a highly reversible discharge capacity of 235.9 mAh g −1 even at a high current density of 10 A g −1 . Thus, VPO@N-G can be applied as a high-rate anode material for sodium-ion batteries.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米复合材料 · 无机功能材料
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Small · 2019 ·Vol. 15 ·期 10 ·1804546 · IF 10.856

Cobalt Phosphides Nanocrystals Encapsulated by P-Doped Carbon and Married with P-Doped Graphene for Overall Water Splitting

Jing Yang,Donghua Guo,Shulin Zhao,Yue Lin,Rui Yang,Dongdong Xu,Naien Shi,Xiaoshu Zhang,Lingzhi Lu,Ya-Qian Lan,Jianchun Bao,Min Han

As one class of important functional materials, transition metal phosphides (TMPs) nanostructures show promising applications in catalysis and energy storage fields. Although great progress has been achieved, phase-controlled synthesis of cobalt phosphides nanocrystals or related nanohybrids remains a challenge, and their use in overall water splitting (OWS) is not systematically studied. Herein, three kinds of cobalt phosphides nanocrystals encapsulated by P-doped carbon (PC) and married with P-doped graphene (PG) nanohybrids, including CoP@PC/PG, CoP-Co 2 P@PC/PG, and Co 2 P@PC/PG, are obtained through controllable thermal conversion of presynthesized supramolecular gels that contain cobalt salt, phytic acid, and graphene oxides at proper temperature under Ar/H 2 atmosphere. Among them, the mixed-phase CoP-Co 2 P@PC/PG nanohybrids manifest high electrocatalytic activity toward both hydrogen and oxygen evolution in alkaline media. Remarkably, using them as bifunctional catalysts, the fabricated CoP-Co 2 P@PC/PG || CoP-Co 2 P@PC/PG electrolyzer only needs a cell voltage of 1.567 V for driving OWS to reach the current density at 10 mA cm −2 , superior to their pure-phase counterparts and recently reported bifunctional catalysts based devices. Also, such a CoP-Co 2 P@PC/PG || CoP-Co 2 P@PC/PG device exhibits outstanding stability for OWS. This work may shed some light on optimizing TMPs nanostructures based on phase engineering, and promote their applications in OWS or other renewable energy options.

研究领域: 材料科学 · 电催化 · 能源化学 · 纳米材料 · 可再生能源
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ChemSusChem · 2019 ·Vol. 12 ·期 4 ·858-865 · IF 7.804

Pyridinic Nitrogen-Doped Graphene Nanoshells Boost the Catalytic Efficiency of Palladium Nanoparticles for the N-Allylation Reaction

Xinxin Li,Qingshan Zhao,Xiang Feng,Lei Pan,Zhuangzhuang Wu,Xiaocui Wu,Tianwen Ma,Jialiang Liu,Yuanyuan Pan,Yan Song,Mingbo Wu

Graphical Nitrogen-doped graphene nanoshells supporting palladium nanoparticles (Pd/N-GNS) have been developed as a superior catalyst for the N -allylation reaction. Experimental results and DFT calculations reveal strong metal–support interactions between the pyridinic N and palladium species, which significantly boost the catalytic efficiency and stability of the catalyst. In this study, nitrogen-doped graphene nanoshells (N-GNS) were developed to support palladium nanoparticles (Pd/N-GNS) as an efficient and recyclable catalyst for the N -allylation reaction. N-GNS was synthesized through a facile hard-template method by using petroleum asphalt, followed by nitrogen doping by thermal annealing with urea, the contents and species of which could be altered by the calcination temperature. Palladium nanoparticles (Pd NPs) with an average diameter of 3.3 nm were homogeneously deposited onto the N-GNS support through a mild solvent-growth approach. The Pd/N-GNS exhibited a superior activity towards the N -allylation reaction, 6-fold higher than that of the pristine graphene nanoshells supporting the palladium catalyst. The Pd/N-GNS could be recycled several times without activity deterioration and metal leaching. The catalytic activity showed a linear correlation relationship with the pyridinic N content. Experimental and theoretical studies reveal strong metal–support interactions between the pyridinic N and palladium species, which can downsize the Pd NPs, modulate the electronic properties, and promote the adsorption of reactant, thereby significantly boosting the catalytic efficiency and stability for the N -allylation process. The present work could help unravel the roles of nitrogen-doped carbon supports and provides a feasible strategy to rationally design superior palladium catalysts for chemical transformations.

研究领域: 材料科学 · 催化化学
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Small · 2023 ·Vol. 20 ·期 17 ·2308632 · IF 13.3

Stable Aluminum Metal Anode Enabled by Dual-Functional Molybdenum Nanoparticles

Shunlong Ju,Qing Qiao,Tian Xu,Zhongchen Zhao,Tengfei Zhang,Guanglin Xia,Xuebin Yu

Constructing robust anode with strong aluminophilicity and rapid desolvation kinetics is essential for achieving high utilization, long-term durability, and superior rate performance in Al metal-based energy storage, yet remains largely unexplored. Herein, molybdenum nanoparticles embedded onto nitrogen-doped graphene (Mo@NG) are designed and prepared as Al host to regulate the deposition behavior and achieve homogeneous Al plating/stripping. The monodispersed Mo nanoparticles reduce the desolvation energy barrier and promote the deposition kinetics of Al. Additionally, Mo nanoparticles act as aluminophilic nucleation sites to minimize the Al nucleation overpotential, further guiding uniform and dense Al deposition. As a result, the dual-functional Mo@NG endows Al anodes with low voltage hysteresis, reversible Al plating/stripping with high coulombic efficiency, and excellent high-rate capability under 5 mA cm −2 . Moreover, the as-designed Al metal full batteries deliver a high capacity retention of 92.8% after 3000 cycles at 1 A g −1 . This work provides an effective solution to optimize the electrochemical properties of Al metal anode from the perspective of desolvation and deposition reactions, towards the development of high-safety and long-cycling aluminum-ion batteries.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米技术 · 金属负极 · 电池化学 · 界面工程
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Nano Energy · 2019 · IF 15.548

Elevated polysulfide regulation by an ultralight all-CVD-built ReS2@N-Doped graphene heterostructure interlayer for lithium–sulfur batteries

Nan Wei,Jingsheng Cai,Ruochen Wang,Menglei Wang,Wei Lv,Haina Ci,Jingyu Sun,Zhongfan Liu

Lithium–sulfur battery is amongst the most promising next-generation energy storage technology owing to their high theoretical capacity and energy density . Nevertheless, the notorious shuttle effect of lithium polysulfides (LiPSs) seriously impedes its practical applications. Here, we report an all-CVD approach to realize the direct growth of ReS 2 @N-doped graphene (NG) heterostructure , which serves as an ultralight high-performance interlayer for elevated LiPS regulation via easy transfer onto the commercial separator. In contrast to the traditional interlayers constructed via vacuum filtration of nanostructured materials that inevitably increase the thickness and weight of the separator, our all-CVD-enabled ReS 2 @NG film possesses an area of 15 mm × 100 mm, a thickness of ~0.5 μm and a negligible areal weight of 80–90 μg cm −2 . Benefiting from the two-dimensional (2D) vertically-erected nanostructure , adsorptive ReS 2 -conductive NG interface, and favorable electrical conductivity , thus-derived ReS 2 @NG interlayer readily enhances reaction kinetics for LiPS conversion and boosts the reutilization of trapped LiPS whilst guaranteeing smooth transportation of lithium ions . Accordingly, an initial discharge capacity of 854 mAh g −1 with an average capacity decay of 0.064% per cycle after 800 cycles can be harvested at 2.0 C. Even at a high sulfur loading of 6.4 mg cm −2 , an initial areal capacity of 6.1 mAh cm −2 can be gained, which still retains 5.8 mAh cm −2 after 40 cycles at 0.1 C. This work is anticipated to shed light upon the construction of CVD-enabled versatile 2D heterostructures for enriching the interlayer design with multifunctionality and cost-effectiveness.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 界面工程 · 电池技术
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