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ADVANCED MATERIALS · 2023 · IF 29.4

Distinguished Roles of Nitrogen-Doped Sp2 and Sp3 Hybridized Carbon on Extraordinary Supercapacitance in Acidic Aqueous Electrolyte

Jun Li,Zhenhai Xia,Xiaowei Wang,Cheng Feng,Qingcheng Zhang,Xi'an Chen,Yun Yang,Shun Wang,Huile Jin

The acidic aqueous supercapacitors have been found to deliver appealing capacitive properties due to fast ion diffusion caused by the applied smallest size of hydrion. However, their practical applications are largely inhibited by the narrow electrochemical stability window of water (1.23 V). Herein, A nitrogen-enriched porous carbon materials (RNOPCs) is reported, consisting of varied nitrogen doping bonded on sp 2 and sp 3 carbon sites, which are capable of stimulating a wider potential window up to 1.4 V and thus resulting in a great enhancement of capacitive performance in aqueous acidic electrolytes. Together with the improved electrical conductivity and preferable hydrion diffusion, RNOPCs exhibit an ultrahigh volumetric capacitance (1084 F cm −3 ) in 0.5 M H 2 SO 4 . Besides, a fully packed RNOPCs-based symmetrical supercapacitor can deliver a high gravimetric and volumetric energy density of 31.8 Wh Kg −1 and 54.3 Wh L −1 respectively, approaching those of lead acid batteries (25–35 Wh Kg −1 ). The first-principles calculations reveal that the lone pair electrons of the doped nitrogen can be delocalized on its neighboring carbon atoms, improving charge uptakes and overpotentials. Such facile and scale-up production of carbon-based supercapacitors can bridge the gap of energy density between traditional supercapacitors and batteries in aqueous electrolytes.

研究领域: 材料科学 · 能源存储与转换
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Joule · 2022 · IF 46.048

A high-voltage and stable zinc-air battery enabled by dual-hydrophobic-induced proton shuttle shielding

Yang-feng Cui,Yun-hai Zhu,Jia-yi Du,Yong-lai Zhang,Kai Li,Wan-qiang Liu,Gang Huang,Xin-bo Zhang

Rechargeable zinc-air batteries (ZABs) stand out among next-generation battery technologies due to their high energy density and high safety but suffer from electrochemical irreversibility. Herein, we report a hybrid ZAB with a long lifespan and high working voltage; it uses a neutral anolyte, an acidic catholyte, and a proton-shuttle-shielding dual-hydrophobic membrane to isolate the two electrolytes. The hybrid ZAB operates through the stable electrochemical plating and stripping of zinc (Zn) in a neutral anolyte and a high-voltage O 2 redox reaction in acidic catholyte. The designed proton-shuttle-shielding dual-hydrophobic membrane selectively transports hydrophobic bis(trifluoromethylsulfonyl)imide anions (TFSI − ) and effectively avoids the crossover of protons. As a result, the hybrid ZAB exhibits a high working voltage (1.50 V) and stable operation (up to 2,000.0 h) in ambient air. This strategy not only overcomes the severe irreversibility of conventional ZABs but also promotes development of electrolyte-decoupled systems.

研究领域: 材料科学 · 电化学
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Nano Select · 2021 ·Vol. 2 ·期 11 ·2126-2134 · IF 0

Stable Pt atomic clusters on carbon nanotubes grafted with carbon quantum dots as electrocatalyst for H2 evolution in acidic electrolyte

Junwei Liang,Yuxiang Liu,Rongzheng Liu,Sufan Zheng,Zhichun Si,Duan Weng,Feiyu Kang

Preparing stable highly dispersed Pt based electrocatalyst is promising to reduce material expense of H 2 product via electrocatalytic water splitting. However, it is still a great challenge to obtain stable single atomic Pt catalysts which can be applied in acidic electrolyte. In the present work, we synthesized Pt atomic clusters on carbon quantum dots (CQDs) grafting multiwall carbon nanotube (CNT) (Pt content: 1 wt.%) catalysts and then loading the catalysts on carbon cloth (Pt content: 0.01 mg▪cm –2 ) for activity test. The overpotential of 29 mV versus RHE was obtained over 1%Pt/CQDs/CNT catalysts at the current density of 10 mA▪cm –2 , and the Tafel slope of 22 mV decade –1 was obtained, too. Especially, the catalysts showed significant stability in hydrogen evolution reactions (HER) in acidic solution, of which the overpotential was still smaller than that of 20%Pt/C after 10,000 CV cycles. CQDs provided coordinating sites for dispersing Pt atomic clusters and improved the H + concentration in adjacent area around the Pt clusters. This method provides a general strategy to design the highly efficient electrocatalysts with ultra-low precious metals for H 2 evolution in acidic electrolyte.

研究领域: 材料科学 · 电化学 · 纳米技术 · 能量转换 · 催化
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IONICS · 2025 · IF 2.6

Synergistic regulation of electronic structure and nanosheet morphology in Ru-doped WS2 for high-efficiency hydrogen evolution reaction

Huang Xiaoyu,Zhang Yaowen,Yang Jian,Xiao Zhizhong,Lu Huidan,Liu Yongping

The synergistic modulation of both the surface electronic configuration and micromorphology of the catalyst is crucial for its electrochemical hydrogen evolution activity. This research successfully developed an efficient Ru-WS 2 NS/CC electrocatalyst for the hydrogen evolution reaction (HER) using a simple two-step strategy involving a solvothermal reaction followed by chemical vapor deposition. The catalyst exhibits excellent electrocatalytic activity and remarkable stability in acidic electrolyte, demonstrating an overpotential of 128.8 mV (at 10 mA cm − 2 ), a Tafel slope of 58.7 mV dec − 1 , and a low charge transfer resistance of only 3.8 Ω, while maintaining high catalytic activity for at least 24 h under acidic conditions. The enhanced HER performance of the Ru-WS 2 NS/CC catalyst is attributed to two main factors: first, the strong electronic interaction induced by Ru doping, which improves the intrinsic electrocatalytic activity; second, the uniform and thin nanosheet morphology of WS 2 provides a highly developed surface area that facilitates hydrogen adsorption and desorption. Density functional theory (DFT) simulations further indicate that introducing Ruthenium (Ru) dopants substantially lowers the Gibbs free energy (ΔG H* ) associated with hydrogen adsorption on the catalyst. Analysis of charge density differences corroborates that such doping strategy efficiently tailors the electronic configuration of the WS 2 support, thereby optimizing its interfacial characteristics. This work proposes an effective electronic structure modulation strategy for developing three-dimensional materials into high-efficiency hydrogen evolution electrocatalysts.

CAS / MDL: 10049-08-8 31175-20-9
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Chem · 2019 · IF 18.205

Photoelectrochemical Synthesis of Ammonia on the Aerophilic-Hydrophilic Heterostructure with 37.8% Efficiency

Jianyun Zheng,Yanhong Lyu,Man Qiao,Ruilun Wang,Yangyang Zhou,Hao Li,Chen Chen,Yafei Li,Huaijuan Zhou,San Ping Jiang,Shuangyin Wang

Photoelectrochemical nitrogen reduction reaction can provide a useful source of ammonia and transportable carrier of hydrogen, but the process is limited by the photocathodes with poor conversion efficiency and low production rate. Here, we have designed a unique aerophilic-hydrophilic heterostructured Si-based photocathode for nitrogen-to-ammonia fixation in an acid electrolyte under mild conditions, achieving a high ammonia yield rate of ∼18.9 μg⋅cm −2 ⋅hr −1 and an excellent faradic efficiency of 37.8% at −0.2 V versus a reversible hydrogen electrode. The heterostructure based on the Au nanoparticles highly dispersed in poly(tetrafluoroethylene) porous framework enriches nitrogen molecular concentration at the Au active sites while manipulateing the proton activity with suppressed hydrogen evolution reactions. DFT calculation indicates that such heterostructure reduces the energy barrier for the nitrogen reduction reaction. The aerophilic-hydrophilic heterostructure provides a new insight on designing efficient and robust photocathodes for nitrogen fixation.

研究领域: 电化学 · 材料科学 · 催化化学 · 能源化学 · 半导体物理 · 纳米科技
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2025 · IF 8.3

Hollow nanosphere Fe-Cu-Co trimetallic selenides with high catalytic performances for hydrogen evolution reaction in both acidic and alkaline electrolytes

Yu Ma,Haitao Zhang,Haizhou Zhang,Xinyuan Ren,Xiaochun Ma,Xiaoming Zhou,Yanlu Mu,Jiemei Yu,Taizhong Huang

Developing non-precious metal based catalysts is one of the most feasible ways to accelerate the application of hydrogen production technology by full water electrolysis with low-cost and high efficiency. In this work, hollow nanosphere structured Fe–Cu–Co trimetallic selenide based catalysts were successfully prepared by one-step hydrothermal method. The hollow nano-spherical shell structure was examined by using XRD, Raman, BET, SEM, TEM, XPS, etc. technologies. The catalytic performance for hydrogen evolution reaction (HER) of the catalysts was tested by LSV, Tafel, CV, EIS, i-t , etc . methods. The overpotential of FeCo 0.1 Cu 0.9 Se 2 catalyzed HER was only 191 (alkaline) and 112 mV (acidic) at 10 mA/cm 2 . The corresponding Tafel slope for HER is 180 mV/dec (alkaline) and 110 mV/dec (acidic), respectively. In addition, the FeCo 0.1 Cu 0.9 Se 2 also showed excellent long-time running stability. The current decay after continuous running 12 h in 0.5 M H 2 SO 4 and 0.1 M KOH electrolytes are 0.07 % and 0.271 %, respectively. FeCo 0.1 Cu 0.9 Se 2 catalyst with the hollow nanospherical structure exhibited excellent catalytic activity for HER. Density functional theory calculations show that the introduction of Co and Cu adjusted the electronic structure of FeCo 0.1 Cu 0.9 Se 2 and the special hollow nano-spherical structure provides enough active catalytic sites for HER. The nano-spherical structured multi-metal selenides show great potential to be high performance catalysts for HER in both alkaline and acidic electrolytes.

研究领域: 材料科学 · 电化学 · 纳米催化 · 能源材料 · 物理化学
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