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Synergy of phosphorus vacancies and build-in electric field into NiCo/NiCoP Mott-Schottky integrated electrode for enhanced water splitting performance

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Chinese Chemical Letters 2024年第2期35卷 604-610页

作者： Xiaochen Zhang Hui Xue Jing Sun Niankun Guo Tianshan Song Jiawen Sun Yi-Ru Hao Qin Wang College of Chemistry and Chemical Engineering Inner Mongolia UniversityHohhot 010021China

Vacancy engineering and Mott-Schottky heterostructure can accelerate charge transfer,regulate adsorption energy of reaction intermediates,and provide additional active sites,which are regarded as valid means for improving catalytic activity.However,the underlying mechanism of synergistic regulation of interfacial charge transfer and optimization of electrocatalytic activity by combining vacancy and Mott-Schottky junction remains unclear.Herein,the growth of a bifunctional NiCo/NiCoP Mott-Schottky electrode with abundant phosphorus vacancies on foam nickel(NF)has been synthesized through continuous phosphating and reduction processes.The obtained NiCo/NiCoP heterojunctions show remarkable OER and HER activities,and the overpotentials for OER and HER are as low as 117 and 60 mV at 10 mA/cm^(2) in 1 mol/L KOH,respectively.Moreover,as both the cathode and anode of overall water splitting,the voltage of the bifunctional NiCo/NiCoP electrocatalyst is 1.44 V at 10 mA/cm^(2),which are far exceeding the benchmark commercial electrodes.DFT theoretical calculation results confirm that the phosphorus vacancies and build-in electric field can effectively accelerate ion and electron transfer between NiCo alloy and NiCoP semiconductor,tailor the electronic structure of the metal centers and lower the Gibbs free energy of the intermediates.Furthermore,the unique self-supported integrated structure is beneficial to facilitate the exposure of the active site,avoid catalyst shedding,thus improving the activity and structural stability of NiCo/NiCoP.This study provides an avenue for the controllable synthesis and performance optimization of Mott-Schottky electrocatalysts.

关键词： Mott-Schottky Build-in electric field Phosphorus vacancies phosphides Overall water splitting

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Bifunctional Electrocatalysts Based on Mo-Doped NiCoP Nanosheet Arrays for Overall Water Splitting

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Nano-Micro Letters 2019年第4期11卷 7-17页

作者： Jinghuang Lin Yaotian Yan Chun Li Xiaoqing Si Haohan Wang Junlei Qi Jian Cao Zhengxiang Zhong Weidong Fei Jicai Feng State Key Laboratory of Advanced Welding and Joining Harbin Institute of TechnologyHarbin 150001People’s Republic of China School of Materials Science and Engineering Harbin Institute of TechnologyHarbin 150001People’s Republic of China MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage State Key Laboratory of Urban Water Resource and EnvironmentSchool of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001People’s Republic of China

Rational design of efficient bifunctional electrocatalysts is highly imperative but still a challenge for overall water splitting.Herein,we construct novel freestanding Mo-doped NiCoP nanosheet arrays by the hydrothermal and phosphation processes,serving as bifunctional electrocatalysts for overall water splitting.Notably,Mo doping could effectively modulate the electronic structure of NiCoP,leading to the increased electroactive site and improved intrinsic activity of each site.Furthermore,an electrochemical activation strategy is proposed to form Mo-doped(Ni,Co)OOH to fully boost the electrocatalytic activities for oxygen evolution reaction.Benefiting from the unique freestanding structure and Mo doping,Mo-doped NiCoP and(Ni,Co)OOH show the remarkable electrochemical performances,which are competitive among current researches.In addition,an overall water splitting device assembled by both electrodes only requires a cell voltage of 1.61 V to reach a current density of 10 mA cm?2.Therefore,this work opens up new avenues for designing nonprecious bifunctional electrocatalysts by Mo doping and in situ electrochemical activation.

关键词： Water splitting Bifunctional electrocatalyst Electronic structure Freestanding Metal phosphides

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Amorphous iron-nickel phosphide nanocone arrays as efficient bifunctional electrodes for overall water splitting

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Green Energy & Environment 2021年第4期6卷 496-505页

作者： Guang Liu Yun Wu Rui Yao Fei Zhao Qiang Zhao Jinping Li Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization College of Chemistry and Chemical EngineeringTaiyuan University of TechnologyTaiyuanShanxi 030024China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China

The synthesis of low-cost and highly active electrodes for both oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is very important for water splitting.In this work,the novel amorphous iron-nickel phosphide(FeP-Ni)nanocone arrays as efficient bifunctional electrodes for overall water splitting have been in-situ assembled on conductive three-dimensional(3D)Ni foam via a facile and mild liquid deposition process.It is found that the FeP-Ni electrode demonstrates highly efficient electrocatalytic performance toward overall water splitting.In 1 M KOH electrolyte,the optimal FeP-Ni electrode drives a current density of 10 mA cm^(-2) at overpotential of 218 mV for the OER and120 mV for the HER,and can attain such current density for 25 h without performance regression.Moreover,a two-electrode electrolyzer comprising the FeP-Ni electrodes can afford 10 mA cm^(-2) electrolysis current at a low cell voltage of 1.62 V and maintain long-term stability,as well as superior to that of the coupled RuO_(2)/NFk Pt/C/NF cell.Detailed characterizations confirm that the excellent electrocatalytic performances for water splitting are attributed to the unique 3D morphology of nanocone arrays,which could expose more surface active sites,facilitate electrolyte diffusion,and benefit charge transfer and also favorable bubble detachment behavior.Our work presents a facile and cost-effective pathway to design and develop active self-supported electrodes with novel 3D morphology for water electrolysis.

关键词： Water splitting Oxygen evolution reaction Hydrogen evolution reaction phosphides Bifunctional electrodes

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Enhancement of the hydrogen evolution performance by finely tuning the morphology of Co-based catalyst without changing chemical composition

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Nano Research 2019年第1期12卷 191-196页

作者： Wenling Gu Liuyong Hu Changshuai Shang Jing Li Erkang Wang State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of Chinese Academy of Sciences Beijing 100049China

Transition-metal phosphides, as the promising alternatives to noble metal catalysts, have been widely used as efficient electrocatalysts for hydrogen evolution reaction (HER). In this work, three kinds of cobalt-8-hydroxyquinoline (Coqx) with different size and nanostructures are synthesized by varying the hydrothermal conditions, which was named as Coqx-L, Coqx-M and Coqx-S according to the decreased size. Accordingly, the CoxP/NC with three different size nanostructures (CoxP/NC-L, CoxP/NC-M and CoxP/NC-S) are obtained by the sequential carbonization and phosphidation of Coqx. The X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) results imply the identical chemical composition in these catalysts with different morphologies. Thus, systematic study is carried out to reveal the relationship between catalytic performance and morphologies of materials with the same chemical composition. The experimental result indicates that the morphology of Cc)xP/NC plays a crucial role on the surface area and electron transfer. Finally, the catalyst of CoxP/NC-S with the smallest size nanostructrue exhibits the best HER performance with a low overpotential at current density of 10 mA/cm^2 (n = 56.9 and 115.6 mV) and a small Tafel slope (52.3 and 69.3 mV/dec) in both 0.1 M HCIO4 and 1.0M KOH as well as long-term stability.

关键词： electrocatalyst hydrogen evolution reaction transition-metal phosphides

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One-pot synthesis of highly conductive nickel-rich phosphide/CNTs hybrid as a polar sulfur host for high-rate and long-cycle Li-S battery

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Nano Research 2019年第5期12卷 1193-1197页

作者： Xiao-Fei Yu Dong-Xu Tian Wen-Cui Li Bin He Yu Zhang Zhi-Yuan Chen An-Hui Lu State Key Laboratory of Fine Chemicals School of Chemical EngineeringDalian University of TechnologyDalian 116024China

Lithium sulfur battery has been identified as a promising candidate for next storage devices attributing to ultrahigh energy density.However,non-conductive nature of sulfur and shuttling effect of soluble lithium polysulfides are intractable remaining problems.Herein,we develop a highly conductive nickel-rich Ni12P5/CNTs hybrid with high specific surface area as sulfur host to address these issues.The polar nature of Ni12Ps/CNTs can significantly relieve the shuttle effect by means of a strong affinity towards lithium polysulfides and enhance kinetics of polysulfides redox reactions.In addition,the Ni12P5/CNTs with a superior conductivity (500 S·m^-1) and high surface area of 395 m^2·g^-1 enables the effective electron transfer and expedited interfacial reaction.As a result,Ni12P5/CNTs hosted sulfur cathode exhibits high rate capability (784 mAh·g^-1 at 4 C) and stable cycling performance with a negligible capacity fading of 0.057 % per cycle over 1,000 cycles at 0.5 C.This work paves an alternative way for designing high performance sulfur cathodes involved metal-rich phosphides.

关键词： Ni-rich phosphides carbon nanotu behigh conductivity catalytic effect lithium sulfur battery

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Surface oxidation of transition metal sulfide and phosphide nanomaterials

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Nano Research 2021年第7期14卷 2264-2267页

作者： Zishan Wu Ling Huang Huan Liu Min Li Hailiang Wang Department of Chemistry Yale UniversityNew HavenConnecticut 06511USA Energy Sciences Institute Yale UniversityWest HavenConnecticut 06516USA Materials Characterization Core Yale West CampusWest HavenConnecticut 06516USA Engineering Laboratory for Next Generation Power and Energy Storage Batteries Tsinghua Shenzhen International GraduateSchoolShenzhen 518055China College of Chemical Engineering Inner Mongolia University of TechnologyHohhot 010051China

Many transition metal sulfides and phosphides are susceptible to surface oxidation under ambient conditions.The formed surface oxidation layer,which is likely to further restructure under reaction conditions,alters the chemical properties of the pristine material but has not been well studied.In this work,we for the first time use X-ray photoelectron spectroscopy to quantify the natural surface oxidation of transition metal phosphide and sulfide nanoparticles and employ a simplified Deal-Grove model to analyze the kinetics.We show that CoS2 oxidizes faster than CoS whereas CoP_(2) is more difficult to oxidize compared to CoP,and there exists an inverse correlation between the surface oxidation rate and the Co-S/P distance in the pristine structure.More inclusive investigation unveils different types of surface oxidation behavior:CoS,NiS and FeS are limited by their reactivity with oxygen;CoS2 is the most reactive and its oxidation is governed by oxygen diffusion;CoP_(2) is influenced by both reactivity and diffusion;CoP,Ni_(2)P,Cu_(3)P and MoP exhibit high initial oxidation degrees and the kinetics are not well-defined;MoS2 is largely stable against oxidation.

关键词： sulfides phosphides surface oxidation kinetics X-ray photoelectron spectroscopy(XPS)

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