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Covalently Bonded Ni Sites in Black Phosphorene with electron redistribution for Efficient Metal‑Lightweighted Water Electrolysis

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Nano-Micro Letters 2024年第6期16卷 233-245页

作者： Wenfang Zhai Ya Chen Yaoda Liu Yuanyuan Ma Paranthaman Vijayakumar Yuanbin Qin Yongquan Qu Zhengfei Dai State Key Laboratory for Mechanical Behavior of Materials Xi’an Jiaotong UniversityXi’an 710049People’s Republic of China School of Chemistry and Chemical Engineering Northwestern Polytechnical UniversityXi’an 710072People’s Republic of China SSN Research Centre SSN College of EngineeringChennaiTamil Nadu 603110India

The metal-lightweighted electrocatalysts for water splitting are highly desired for sustainable and economic hydrogen energy deployments,but *** this work,a low-content Ni-functionalized approach triggers the high capability of black phosphorene(BP)with hydrogen and oxygen evolution reaction(HER/OER)*** a facile in situ electro-exfoliation route,the ionized Ni sites are covalently functionalized in BP nanosheets with electron redistribution and controllable metal *** is found that the as-fabricated Ni-BP electrocatalysts can drive the water splitting with much enhanced HER and OER *** 1.0 M KOH electrolyte,the optimized 1.5 wt%Nifunctionalized BP nanosheets have readily achieved low overpotentials of 136 mV for HER and 230 mV for OER at 10 mA cm^(−2).Moreover,the covalently bonding between Ni and P has also strengthened the catalytic stability of the Ni-functionalized BP electrocatalyst,stably delivering the overall water splitting for 50 h at 20 mA cm^(−2).Theoretical calculations have revealed that Ni–P covalent binding can regulate the electronic structure and optimize the reaction energy barrier to improve the catalytic activity *** work confirms that Ni-functionalized BP is a suitable candidate for electrocatalytic overall water splitting,and provides effective strategies for constructing metal-lightweighted economic electrocatalysts.

关键词： Black phosphorus Water electrolysis Electrocatalyst electron redistribution Covalent functionalization

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Tailoring interfacial electron redistribution of Ni/Fe_(3)O_(4) electrocatalysts for superior overall water splitting

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Journal of Energy Chemistry 2022年第10期31卷 330-338,I0008页

作者： Wenli Xu Wenda Zhong Chenfan Yang Rong Zhao Jing Wu Xuanke Li Nianjun Yang Hubei Province Key Laboratory of Coal Conversion and New Carbon Materials Wuhan University of Science and TechnologyWuhan 430081HubeiChina Hunan Province Key Laboratory for Advanced Carbon Materials and Applied Technology Hunan UniversityChangsha 410082HunanChina Institute of Materials Engineering University of SiegenSiegen 57076Germany

Exploring highly active earth-abundant bifu nctional electrocatalysts for water splitting at a high output is essential for the forthcoming hydrogen ***-noble Fe_(3)O_(4) catalyst owns outstanding conductivity and its octahedral Fe sites can markedly promote water ***,it lacks active centers on the surface,resulting in its poor activity when used as a catalyst for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Herein,an electron redistribution strategy is proposed by introducing Ni sites onto the surface of Fe_(3)O_(4)(Ni/Fe_(3)O_(4)).The abundant delocalized electrons,derived from the electronic interaction of Ni and Fe_(3)O_(4) species,significantly optimize the electronic structure of the Ni/Fe_(3)O_(4) catalyst,leading to its improved adsorption *** Ni/Fe_(3)O_(4) catalyst exhibits remarkable bifunctional activity,steadily outputting 1000 mA cm^(-2)at the low overpotential of 387 mV for HER and 338 mV for OER,*** Ni/Fe_(3)O_(4) as a bifunctional catalyst for overall water splitting reaction exhibits the optimal performance with outstanding stability,obtaining a current density of1000 mA cm^(-2)at 1.98 V,much superior to a Pt/C‖IrO_(2)*** analysis and theoretical calculations collectively corroborate that the electron redistribution of Fe_(3)O_(4) is activated by coupling Ni species,leading to the promoted HER and OER *** electron redistribution strategy provides an effective method to activate transition metal-based catalysts which are promising to be utilized as superior electrocatalysts for the industrial overall water splitting reaction.

关键词： electron redistribution Ni/Fe_(3)O_(4)heterojunction Overall water splitting

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Interfacial coupling of sea urchin-like(Mo4O11-MoS2-VO_(2)) promoted electron redistributions for significantly boosted hydrogen evolution reaction

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Chinese Chemical Letters 2023年第4期34卷 368-373页

作者： Yupeng Xing Na Li Shipeng Qiu Gang Zhao Shuhua Hao Baojie Zhang Laboratory of Functional Micro-nano Materials and Devices School of Physics and TechnologyUniversity of JinanJi’nan 250022China

Developing efficient electrocatalysts for hydrogen evolution reaction(HER) is of great importance in contemporary water electrolysis technology. Here, a novel hierarchically sea urchin-like electrocatalyst(Mo_(4)O_(11)-MoS_(2)-VO_(2)) is synthesized by hydrothermal deposition and post-annealing strategy. The optimized electrocatalyst behaves as a high active hydrogen evolution electrode in 0.5 mol/L H_(2)SO_(4). This electrode needs overpotential of only 43 m V to achieve 10 m A/cm^(2)with a Tafel slope of 37 m V/dec and maintains its catalytic activity for at least 36 h. Better than most previously reported non-noble metal electrocatalysts anchored on carbon cloth. It is worth mentioning that the hierarchical sea urchin-like structure promotes the redistribution of electrons and provides more catalytic active sites. This strategy shows a way for the construction of inexpensive non-noble metal electrocatalysts in the future.

关键词： Non-noble metal Hierarchical sea urchin-like (Mo4O11-MoS2-VO_(2)) Interfacial coupling electron redistribution HER

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Self-standing hollow porous Co/a-WO_(x)nanowire with maximum Mott-Schottky effect for boosting alkaline hydrogen evolution reaction

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Nano Research 2023年第4期16卷 4603-4611页

作者： Jianpo Chen Jianping Zheng Weidong He Haikuan Liang Yan Li Hao Cui Chengxin Wang School of Materials Science and Engineering The Key Laboratory of Low-Carbon Chemistry&Energy Conservation of Guangdong ProvinceSun Yatsen UniversityGuangzhou 510275China

The sufficient utilization of Mott-Schottky effect for boosting alkaline hydrogen evolution reaction(HER)depends upon scale minimizing of interface components and exposure maximizing of Mott-Schottky ***,a self-standing porous tubular Mott-Schottky electrocatalyst is constructed by a self-template etching strategy,where amorphous WO_(x)(a-WO_(x))nano-matrix connects Co *** novel“Janus”electrocatalyst maximizes the Mott-Schottky effect by not only providing a highly exposed micro interface,but also simultaneously accelerating the water dissociation and optimizing the hydrogen desorption *** findings and theoretical calculations reveal that Co/a-WO_(x)Mott-Schottky heterointerface triggers the electron redistribution and a build-in electric field,which can not only optimize the adsorption energy of the reaction intermediates,but also facilitate the charge ***,Co/a-WO_(x)requires an overpotential of only 36.3 mV at 10 mA·cm^(−2)and shows a small Tafel slope of 53.9 mV·dec^(−1)as well as an excellent 200-h long-term *** work provides a novel design strategy for maximizing the Mott-Schottky effect on promoting alkaline HER.

关键词： Mott-Schottky effect electrocatalyst self-template etching hydrogen evolution reaction(HER) electron redistribution

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Adsorption Site Regulations of[W–O]‑Doped CoP Boosting the Hydrazine Oxidation‑Coupled Hydrogen Evolution at Elevated Current Density

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Nano-Micro Letters 2023年第11期15卷 418-434页

作者： Ge Meng Ziwei Chang Libo Zhu Chang Chen Yafeng Chen Han Tian Wenshu Luo Wenping Sun Xiangzhi Cui Jianlin Shi Shanghai Institute of Ceramics Chinese Academy of SciencesShanghai 200050People’s Republic of China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049People’s Republic of China State Key Laboratory of Clean Energy Utilization School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China School of Chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024People’s Republic of China

Hydrazine oxidation reaction(HzOR)assisted hydrogen evolution reaction(HER)offers a feasible path for low power consumption to hydrogen *** however,the total electrooxidation of hydrazine in anode and the dissociation kinetics of water in cathode are critically depend on the interaction between the reaction intermediates and surface of catalysts,which are still challenging due to the totally different catalytic ***,the[W–O]group with strong adsorption capacity is introduced into CoP nanoflakes to fabricate bifunctional catalyst,which possesses excellent catalytic performances towards both HER(185.60 mV at 1000 mA cm^(−2))and HzOR(78.99 mV at 10,00 mA cm^(−2))with the overall electrolyzer potential of 1.634 V lower than that of the water splitting system at 100 mA cm^(−2).The introduction of[W–O]groups,working as the adsorption sites for H2O dissociation and N2H4 dehydrogenation,leads to the formation of porous structure on CoP nanoflakes and regulates the electronic structure of Co through the linked O in[W–O]group as well,resultantly boosting the hydrogen production and ***,a proof-of-concept direct hydrazine fuel cell-powered H_(2) production system has been assembled,realizing H_(2)evolution at a rate of 3.53 mmol cm^(−2)h^(−1)at room temperature without external electricity supply.

关键词： Self-powered H_(2)production system electron redistribution [W–O]dopant Dehydrogenation kinetics

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Phosphorus-doped MoS_(2) with sulfur vacancy defects for enhanced electrochemical water splitting

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Science China Materials 2022年第3期65卷 712-720页

作者： Hongyao Xue Alan Meng Chunjun Chen Hongyan Xue Zhenjiang Li Chuansheng Wang College of Electromechanical Engineering Qingdao University of Science and TechnologyQingdao 266061China Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science MOECollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular Sciences Institute of ChemistryChinese Academy of SciencesBeijing 100190China University of Kent Canterbury CT27NZKent CountyUK College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266061China National Engineering Laboratory for Advanced Equipments and Key Materials for Tires Qingdao University of Science and TechnologyQingdao 266042China

MoS_(2)is a promising electrocatalyst because of its natural abundance and outstanding electrochemical ***,the poor conductivity and low activity limit its catalytic performance;furthermore,MoS_(2)is unable to satisfy the requirements of most industrial *** this study,to obtain a P-doped MoS_(2)catalyst with S vacancy defects,P is inserted into the MoS_(2)matrix via a solid phase ion exchange at room *** optimal P-doping amount is 11.4 wt%,and the resultant catalyst delivers excellent electrocatalytic properties for the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)with the corresponding overpotentials of 93 and 316 mV at 10 mA cm^(-2) in an alkaline solution;these values surpass the overpotentials of most previously reported MoS_(2)-based *** calculations and results demonstrate that the synergistic effect of the doped P,which forms active centers in the basal plane of MoS_(2),and S vacancy defects caused by P doping intensifies the intrinsic electronic conductivity and electrocatalytic activity of the *** functional theory calculations demonstrate that P optimizes the free energy of the MoS_(2)matrix for hydrogen adsorption,thereby considerably increasing the intrinsic activity of the doped catalyst for the HER compared with that observed from pristine MoS_(2).The enhanced catalytic activity of P-doped MoS_(2)for the OER is attributed to the ability of the doped P which facilitates the adsorption of hydroxyl and hydroperoxy intermediates and reduces the reaction energy *** study provides a new environmentally friendly and convenient solid-phase ion exchange method to improve the electrocatalytic capability of two-dimensional transition-metal dichalcogenides in largescale applications.

关键词： molybdenum disulfide phosphorus doping sulfur vacancy defects overall water splitting electron redistribution density functional theory calculations

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Nanoporous nickel with rich adsorbed oxygen for efficient alkaline hydrogen evolution electrocatalysis

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Science China Materials 2022年第7期65卷 1825-1832页

作者： Qingfeng Hu Zelin Chen Jiajun Wang Xuerong Zheng Xiaopeng Han Yida Deng Wenbin Hu School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin UniversityTianjin 300072China State Key Laboratory of Marine Resource Utilization in South China Sea School of Materials Science and EngineeringHainan UniversityHaikou 570228China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207China

Sluggish water dissociation kinetics severely limits the rate of alkaline electrocatalytic hydrogen evolution reaction(HER).Therefore,finding highly active electrocatalysts and clarifying the mechanism of water dissociation are challenging but *** this study,we report an integrated nanoporous nickel(np-Ni)catalyst with high alkaline HER performance and the origin of the corresponding enhanced catalytic *** 1 mol L^(-1) KOH solution,this np-Ni electrode shows an HER overpotential of 20 mV at 10 mA cm^(-2),along with fast water dissociation *** excellent performance is not only attributed to the large surface area provided by the three-dimensional interconnected conductive network but also from the enhanced intrinsic activity induced by the unique surface *** studies reveal that the types of oxygen species that naturally form on the Ni surface play a key role in water ***,when the lattice oxygen almost disappears,the Ni surface terminates with_(ads)orbed oxygen(O_(ads)),exhibiting the fastest water dissociation *** functional theory calculation suggests that when O_(ads)acts as the surface termination of Ni metal,the orientation and configuration of polar water molecules are strongly affected by O_(ads).Finally,the H–OH bond of interfacial water molecules is effectively activated in a manner similar to hydrogen *** work not only identifies a high-performance and low-cost electrocatalyst but also provides new insights into the chemical processes underlying water dissociation,thus benefiting the rational design of electrocatalysts.

关键词： alkaline hydrogen evolution water dissociation electron redistribution adsorbed oxygen hydrogen bond

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