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Journal of Materials Chemistry A · 2017 ·Vol. 5 ·期 47 ·24767-24774 · IF 8.867

Hierarchical Ni/NiTiO3 derived from NiTi LDHs: a bifunctional electrocatalyst for overall water splitting

Chenlong Dong,Xiangye Liu,Xin Wang,Xiaotao Yuan,Ziwan Xu,Wujie Dong,Muhammad Sohial Riaz,Guobao Li,Fuqiang Huang

Developing economical and stable bifunctional electrocatalysts for overall water splitting is of enormous importance for sustainable energy systems. Here, Ni/NiTiO3 with a villiform structure assembled by nanosheets is presented as an efficient bifunctional electrocatalyst. The Ni/NiTiO3 with a molar ratio of 15 : 1 (Ni : Ti) manifests remarkable catalytic performance for both the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) in alkaline solutions, with onset overpotentials of 270 mV for the OER and ∼50 mV for the HER. Large amounts of Ni nanoparticles inset in the NiTiO3 nanosheets possess a high specific surface of 28.4 m2 g−1 which is far greater than that of bare Ni (7.7 m2 g−1). The results of long-term OER operation confirm that the introduction of Ti4+ is favorable for enhanced stability. When the catalyst is employed as both the cathode and anode for overall water splitting, it displays an onset potential of 1.55 V in 1 M KOH solution which can rival that of the integrated performance of Pt/C and RuO2. Hence, our Ni/NiTiO3 electrocatalysts have enormous potential for realistic large-scale water splitting.

研究领域: 材料科学 · 能源化学
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Nano Select · 2021 ·Vol. 3 ·期 1 ·147-156 · IF 0

In situ fabrication of cobalt/nickel sulfides nanohybrid based on various sulfur sources as highly efficient bifunctional electrocatalysts for overall water splitting

Mengqiu Li,Ze Xu,Yuting Li,Juan Wang,Qin Zhong

Transition metal chalcogenides are attractive electrocatalysts for oxygen evolution reaction (OER) or hydrogen evolution reaction (HER) due to their natural abundance and diverse structure. Herein, nickel sulfides (Ni 3 S 2 ) and nickel/cobalt sulfides nanohybrid have been in situ fabricated on nickel foam (NF) by a facile hydrothermal method with sodium sulfide (Ss), L-cysteine (Lc) or thiourea (Tu) as a sulfur source, respectively. The results show that sulfur source has a great influence on the phase structure, morphology and electrocatalytic performance of transition metal sulfides. The nickel sulfide with the sodium sulfide as a sulfur source (Ni Ss ) shows better HER and OER activity in 1 M KOH. With the Co-doping, three-dimensional honeycomb-like NiCo Ss nanosheet clusters exhibits the enhanced electrocatalysis properties with overpotentials of only 168 mV at 10 mA cm –2 for HER and 234 mV at 20 mA cm –2 for OER, respectively. The NiCo Ss shows the good bifunctional activities for overall water splitting and presents considerable stability for 24 hours. The good electrochemical activities of metal sulfides by using inorganic sodium sulfide can be attributed to the large exposed surface area and heterostructure compositions of Co 9 S 8 and Ni 3 S 2 .

研究领域: 材料科学 · 电化学 · 能源技术
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Natural DNA-derived highly-graphitic N, P, S-tridoped carbon nanosheets for multiple electrocatalytic applications

Qian Yu,Jingshu Wang,Haibo Li,Ruiqing Li,Suyuan Zeng,Rui Li,Qingxia Yao,Hongyan Chen,Konggang Qu,Yao Zheng

In the electrocatalytic oxygen reduction and hydrogen evolution reactions (ORR/HER), metal-free carbon-based materials presented great potentials as alternatives to Pt because of their flexible adjustability of electronic and geometric properties. The pursuit of high-performance carbons demand for high-level doping, large surface area and high graphitization, but the improvement of the former two aspects would inevitably impair the third one, which seems a contradictive proposition. Herein, by a facile “mix-and-pyrolyze” method, natural DNA was first developed to synthesize N, P, S-tridoped carbons (NPSC) with porous sheet structures, high graphitization, large surface areas and abundant high-quality dopants simultaneously. Thus, the newly-prepared NPSC displays superior alkaline ORR performance comparable to Pt/C together with excellent acidic activity and better stability. Meanwhile, NPSC is one of most active acidic HER catalysts and the best alkaline HER catalyst among carbon counterparts. Density function theory computation reveled the origins of superior performance are attributed to positively charged C sites neighboring to S for ORR and P sites for HER because of DNA-derived advantaged structural features. The as-fabricated rechargeable zinc–air battery based on current tridoped carbon has closed peak power density and specific capacity but much better charge–discharge stability compared with Pt/C.

研究领域: 材料科学 · 电化学 · 计算化学
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RARE METALS · 2024 ·Vol. 43 ·期 11 ·5860-5867 · IF 9.6

Two-dimensional metallic CoTe2 flakes for electrocatalytic hydrogen evolution

Zhao Yu-Qing,Liu Qian,Zhou Bo-Jian,Yang Guang,Jiang Shao-Long

Two-dimensional (2D) metallic 1T-CoTe 2 has attracted considerable attention due to its fascinating physical properties and promising applications in electronics and catalysis. However, the production of high-quality 2D 1T-CoTe 2 still remains challenging. Herein, we demonstrate a methodology to realize the facile synthesis of ultrathin, high-quality CoTe 2 flakes with a thickness down to 2.3 nm on mica substrates by an ambient-pressure chemical vapor deposition (CVD) technique. The atomic arrangement is verified by scanning transmission electron microscopy. The theoretical calculations uncover the metallic characteristic of 1T-CoTe 2 in the 2D limit. Remarkably, the CVD-derived 2D metallic CoTe 2 flakes for the hydrogen evolution reaction (HER) catalyst exhibit admirable performance, such as an overpotential of 186 mV at 10 mA·cm −2 , a Tafel slope of 78 mV·dec −1 , an exchange current density of 69 μA·cm −2 , and negligible performance degradation after 1000 cycles. These results establish novel approaches for the synthesis and HER application of 2D metallic 1T-CoTe 2 . Graphical abstract

研究领域: 材料科学 · 催化化学 · 纳米科技 · 表面科学 · 能源材料
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Small · 2023 ·Vol. 19 ·期 41 ·2302685 · IF 13.3

Boosting the Hydrogen Evolution Reaction Performance of P-Doped PtTe2 Nanocages via Spontaneous Defects Formation

Hancheng Ma,Xiang Huang,Luyu Li,Wei Peng,Sheng Lin,Yao Ding,Liqiang Mai

PtTe 2 , a member of the noble metal dichalcogenides (NMDs), has aroused great interest in exploring its behavior in the hydrogen evolution reaction (HER) due to the unique type-II topological semimetallic nature. In this work, a simple template-free hydrothermal method to obtain the phosphorus-doped (P-doped) PtTe 2 nanocages with abundant amorphous and crystalline interface (A/C-P-PtTe 2 ) is developed. Revealed by density functional theory calculations, the atomic Te vacancies can spontaneously form on the basal planes of PtTe 2 by the P doping, which results in the unsaturated Pt atoms exposed as the active sites in the amorphous layer for HER. Owing to the defective structure, the A/C-P-PtTe 2 catalysts have the fast Tafel step determined kinetics in HER, which contributes to an ultralow overpotential ( η = 28 mV at 10 mA cm −2 ) and a small Tafel slope of 37 mV dec −1 . More importantly, benefiting from the inner stable crystalline P-PtTe 2 nanosheets, limited decay of the performance is observed after chronopotentiometry test. This work reveals the important role of the inherent relationship between structure and activity in PtTe 2 for HER, which may bring another enlightenment for the design of efficient catalysts based on NMDs in the near future.

研究领域: 材料科学 · 电化学 · 纳米催化 · 能源材料 · 计算材料学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Achieving an efficient hydrogen evolution reaction with a bicontinuous nanoporous PtNiMg alloy of ultralow Noble-metal content at an ultrawide range of current densities

Yuexi Zheng,Pengfei Shang,Feng Pei,Guang Ma,Zhiguo Ye,Xinyuan Peng,Duosheng Li

Electrochemical water splitting powered by green electricity generated from intermittent geothermal, wind and solar power is a promising approach to realize large-scale hydrogen production owing to its sustainable and clean characteristics. Developing electrocatalysts with high electrocatalytic activity and long-term stability for the hydrogen evolution reaction (HER) at an ultrahigh current density (>1000 mA cm −2 ) still needs a breakthrough. Here, a bicontinuous nanoporous PtNiMg alloy with an ultralow noble metal content for the HER is fabricated by a facile high-temperature sintering method based on the nanoscale Kirkendall effect. A bicontinuous nanoporous alloy electrode with an ultralow content of approximately 1 at % Pt for the HER in an alkaline medium achieves an extremely low overpotential of 22 mV at a current density of 10 mA cm −2 and a Tafel slope (30.9 mV dec -1 ) of the Volmer-Tafel mechanism. The alloy electrode for the HER at a wide current density of 1–2000 mA cm −2 displays superior stability in alkaline media. The 3D bicontinuous nanoporous structure, perfect synergistic effect of Ni and Pt species, high structural stability and excellent conductivity of the 1-PtNiMg-900 alloy achieve outstanding electrocatalytic activity and long-term stability at an ultrawide range of HER current densities. This study greatly improves the electrochemical performance of Pt-based electrocatalysts for the HER via a novel fabrication approach and provides the possibility of large-scale industrial application for H 2 production.

研究领域: 材料科学 · 电化学 · 纳米科技 · 能源化学 · 催化化学
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MATERIALS & DESIGN · 2016 · IF 3.997

Carbon nanofibers as nanoreactors in the construction of PtCo alloy carbon core-shell structures for highly efficient and stable water splitting

XinRong Liu,Ming Zhang,TingTing Yang,LiNa Wang,Han Zhu,ShunLi Wang,MingLiang Du

Carbon nanofibers served as nanoreactors for the design and construction of PtCo alloy carbon core-shell nanostructures with nitrogen doping (PtCo/NCNF) through a combination of electrospinning and nitrogen doping treatments. The PtCo/NCNF hybrid consists of PtCo alloy nanoparticles surrounded by a few of N-doped carbon layers , demonstrating a typical core-shell structures. The PtCo/NCNF hybrid can both served as electrode materials for electrocatalytic water splitting including hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). For the HER performance, the PtCo/NCNF exhibits very small onset potential of 20   mV, an overpotential of 50   mV at a j (vs RHE)   =   10   mA   cm −   2 and Tafel slope of 30   mV   dec −   1 . The PtCo/NCNF hybrid also exhibits high OER activity with an onset potential of 310   mV, an overpotential of 400   mV at a j of 10   mA   cm −   2 and a small Tafel slope of 76   mV   dec −   1 . The high catalytic activities of PtCo alloy for HER and OER originate from the 3D hierarchical structures, well-dispersed PtCo alloy, high conductivity of NCNF, protection from the carbon-encapsulated structure, and the introduction of nitrogen.

研究领域: 材料科学 · 纳米技术 · 电化学 · 能源化学 · 催化化学 · 功能材料
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Frontiers in Chemistry · 2022 · IF 5.545

Tannic acid assisted metal–chelate interphase toward highly stable Zn metal anodes in rechargeable aqueous zinc-ion batteries

Nan Hu,Hongyu Qin,Xiangyou Chen,Yanping Huang,Jing Xu,Huibing He

Aqueous zinc-ion batteries (AZIBs) have attracted extensive attention because of their eco-friendliness, intrinsic safety, and high theoretical capacity. Nevertheless, the long-standing Zn anode issues such as dendrite growth, hydrogen evolution, and passivation greatly restrict the further development of AZIBs. Herein, a metal–chelate interphase with high Zn affinity is constructed on the Zn metal surface (TA@Zn) via dipping metallic Zn into a tannic acid (TA) solution to address the aforementioned problems. Benefiting from the abundant hydrophilic and zincophilic phenolic hydroxyl groups of TA molecules, the metal–chelate interphase shows strong attraction for Zn2+ ions, guiding uniform zinc deposition as well as decreasing Zn2+ migration barrier. Therefore, the TA@Zn anode displays an extended lifespan of 850 h at 1 mA cm−2, 1 mAh cm−2 in the Zn|Zn symmetrical cell, and a high Coulombic efficiency of 96.8% in the Zn|Ti asymmetric cell. Furthermore, the Zn|V2O5 full cell using TA@Zn anode delivers an extremely high capacity retention of 95.9% after 750 cycles at 2 A g−1. This simple and effective strategy broadens the interfacial modification scope on Zn metal anodes for advanced rechargeable Zn metal batteries.

研究领域: 电化学 · 材料科学 · 能源存储 · 界面化学 · 金属负极 · 电池技术
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CHINESE JOURNAL OF CATALYSIS · 2021 ·Vol. 42 ·期 10 ·1798-1807 · IF 8.271

Controlling atomic phosphorous-mounting surfaces of ultrafine W2C nanoislands monodispersed on the carbon frameworks for enhanced hydrogen evolution

Xiangyong Zhang,Tianying Liu,Ting Guo,Xueying Han,Zongyun Mu,Qiang Chen,Jiangmin Jiang,Jing Yan,Jiaren Yuan,Dezhi Wang,Zhuangzhi Wu,Zongkui Kou

Controllably mounting foreign atoms on the surfaces of earth-abundant electrocatalysts strongly improve their surface electronic properties for optimizing the catalytic performance of surficial sites to an unusual level, and provides a good platform to gain deep insights into catalytic reactions . The present work describes, employing ultrafine W 2 C nanoislands (average size: 2.3 nm) monodispersed on the N, P dual-doped carbon frameworks as a model system, how to regulate the atomic phosphorous-mounting effect on the surfaces of W 2 C to derive an active and stable P-mounting W 2 C (WCP) catalyst for both acidic and alkaline hydrogen evolution reaction (HER). Since in situ phosphorus substitution into carbon sites of preformed W 2 C nanoislands gradually proceeds from surfaces to solids, so that using a proper amount of phosphorus sources can readily control the surface mounting level to avoid the mass P-doping into the bulk. By this way, the activity per active site of WCP catalyst with robust stability can be optimized to 0.07 and 0.56 H 2 s −1 at –200 mV overpotential in acid and base, respectively, which reach up to the several-fold of pure-phase W 2 C (0.01 and 0.05 H 2 s −1 ). Theoretical investigations suggest that compared with solid P doping, the P mounting on W 2 C surface can more remarkably enhance its metallicity and decrease the hydrogen release barrier. This finding disclosed a key correlation between surface foreign atom-mounting and catalytic activity , and suggested a logical extension to other earth-abundant catalysts for various catalytic reactions .

研究领域: 材料化学 · 电催化 · 纳米材料 · 能源科学 · 表面科学 · 理论计算
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ELECTROCHIMICA ACTA · 2018 · IF 5.116

Polyvinyl alcohol protected Mo2C/Mo2N multicomponent electrocatalysts with controlled morphology for hydrogen evolution reaction in acid and alkaline medium

Xiaozhen Chen,Ji Qi,Pan Wang,Chuang Li,Xiao Chen,Changhai Liang

Herein, PVA-Mo 2 C/Mo 2 N nanospheres with surface roughness are synthesized via a polyvinyl alcohol (PVA) involved approach and used for hydrogen evolution reaction (HER). The average crystallite size of the PVA protected nMo 2 CN nanospheres (6.1 nm) is one third of that of the PVA-Mo 2 C/Mo 2 N without PVA protection (17.9 nm). At 10 mA cm −2 current density, the as-synthesized PVA-Mo 2 C/Mo 2 N nanospheres with surface roughness exhibit HER overpotentials of 132 mV and 142 mV with corresponding Tafel slope of 51.8 mV dec −1 and 50.4 mV dec −1 in acid and alkaline medium, respectively. This high apparent activity can be attributed to the high intrinsic activity originated from the adjacent surface active sites of Mo 2 C and Mo 2 N as well as the large ECSA of PVA-Mo 2 C/Mo 2 N nanospheres with surface roughness.

研究领域: 材料科学 · 电化学 · 纳米催化 · 能源化学 · 表面科学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Directly anchoring non-noble metal single atoms on 1T-TMDs with tip structure for efficient hydrogen evolution

Wenda Zhou,Zhenzhen Jiang,Mingyue Chen,Zhaohui Li,Xingfang Luo,Manman Guo,Yong Yang,Ting Yu,Cailei Yuan,Shouguo Wang

Owing to tip effect can introduce localized enhanced electric field and reduce interfacial energy barrier, design of atomic tip structure in single-atom catalysts (SACs) may be a fascinating strategy to further improve its electrocatalytic activity. However, conventional synthesis methods, such as defect-trapping or substitution, only lead to the formation of planar geometry of SACs without tip atoms. Good conductive 1T-TMDs with electrocatalytically active basal plane can provide platform to directly stabilize single atoms (SAs) on the top sites of its surface to form atomic tip structure. Herein, a universal Laser-molecular beam epitaxy (L-MBE) method for precisely controlling non-noble metal SAs directly immobilizing on the Cr top site of 1T-CrS 2 metallic basal plane is developed. In case of Mo, the Mo SAs@1T-CrS 2 with single-atom tip structure can exhibit enhanced electric field surrounding Mo atoms and an almost zero hydrogen adsorption free energy, resulting in superior HER performance together with high stability. This work provides a general way to design varieties of SACs in widely catalytic application.

研究领域: 材料科学 · 电化学 · 纳米催化 · 能源材料 · 表面科学
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Small · 2024 ·Vol. 21 ·期 4 ·2410657 · IF 13

2D MOF Structure Tuning Atomic Ru Sites for Efficient and Robust Proton Exchange Membrane Water Electrolysis

Jia Wang,De Wang,Zelin Zhao,Ganggang Chang,Wei Guo,Jun Xu,Yinyu Xiang,Junrui Li,Junsheng Li

Developing cost-effective ruthenium (Ru)-based HER electrocatalysts as alternatives to commercial Pt/C is crucial for the advancement of proton exchange membrane water electrolysis (PEMWE). However, the strong hydrogen adsorption of Ru-based catalysts restricts its activity. Herein, a strategy is reported to tune the electronic structure and improve mass transfer by implanting Ru atoms onto the (002) facet of two-dimensional zeolitic imidazolate framework-67 (Ru@ L ZIF (002) ) to optimize the d -band center ( ε d ) of Ru and the hydrogen spillover behavior. Benefiting from the ultrathin nanosheet structure and optimized ε d of Ru, the over-strong H adsorption energy is weakened and the electron/mass transfer is facilitated. Ru@ L ZIF (002) exhibits an overpotential of 9.2 mV at 10 mA cm −2 and a long-lasting stability of 35 days at 100 mA cm −2 . The mass activity and price activity of Ru@ L ZIF (002) is 2.9 and 14.7 times higher than Pt/C, respectively. More impressively, Ru@ L ZIF (002) delivers a cell voltage of 2.01 V at a high current density of 4 A cm −2 in PEMWE. The excellent long-term durability of 1200 hours operating at 4 A cm −2 with an ultralow decay rate of 7.5 × 10 −3 mV h −1 has been achieved, making it promising as a cost-effective alternative to Pt/C catalyst for PEMWE applications.

研究领域: 电催化 · 材料科学 · 能源化学 · 纳米材料 · 电化学工程 · 可持续能源技术
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