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Nitrogen vacancies enriched Ce-doped Ni_(3)N hierarchical nanosheets triggering highly-efficient urea oxidation reaction in urea-assisted energy-saving electrolysis

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Journal of Energy Chemistry 2022年第6期31卷 506-515,I0014页

作者： Meng Li Xiaodong Wu Kun Liu Yifan Zhang Xuechun Jiang Dongmei Sun Yawen Tang Kai Huang Gengtao Fu Jiangsu Key Laboratory of New Power Batteries Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023JiangsuChina School of Chemistry and Chemical Engineering Southeast UniversityNanjing 211189JiangsuChina College of Materials Science and Engineering Nanjing Tech UniversityNanjing 210009JiangsuChina

urea oxidation reaction (UOR),which has favorable thermodynamic energy barriers compared with oxygen evolution reaction (OER),can provide more cost-effective electrons for the renewable energy systems,but is trapped by its sluggish UOR kinetics and intricate reaction intermediates formation/desorption process.Herein,we report a novel and effective electrocatalyst consisting of carbon cloth supported nitrogen vacancies-enriched Ce-doped Ni_(3)N hierarchical nanosheets (Ce-Ni_(3)N @CC) to optimize the flat-footed UOR kinetics,especially the stiff rate-determine CO_(2)desorption step of UOR.Upon the introduction of valance state variable Ce,the resultant nitrogen vacancies enriched Ce-Ni_(3)N @CC exhibits an enhanced UOR performance where the operation voltage requires only 1.31 V to deliver the current density of 10 mA cm^(-2),which is superior to that of Ni_(3)N @CC catalyst (1.36 V) and other counterparts.Density functional theory (DFT) results demonstrate that the incorporation of Ce in Ni_(3)N lowers the formation energy of nitrogen vacancies,resulting in rich nitrogen vacancies in Ce-Ni_(3)N @CC.Moreover,the nitrogen vacancies together with Ce doping optimize the local charge distribution around Ni sites,and balance the adsorption energy of CO_(2)in the rate-determining step (RDS),as well as affect the initial adsorption structure of urea,leading to the superior UOR catalytic performance of Ce-Ni_(3)N @CC.When integrating the Ce-Ni_(3)N catalyst in UOR//HER and UOR//CO_(2)R flow electrolyzer,both of them perform well with low operation voltage and robust long-term stability,proofing that the thermodynamically favorable UOR can act as a suitable substitute anodic reaction compared with that of OER.Our findings here not only provide a novel UOR catalyst but also offer a promising design strategy for the future development of energy-related devices.

关键词： Rare earth cerium Nickel nitride Nitrogen vacancies Charge redistribution urea oxidation reaction

Two-dimensional bimetallic coordination polymers as bifunctional evolved electrocatalysts for enhanced oxygen evolution reaction and urea oxidation reaction

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Journal of Energy Chemistry 2021年第12期30卷 230-238,I0005页

作者： Qiang Li Lele Lu Jingwei Liu Wei Shi Peng Cheng Key Laboratory of Advanced Energy Materials Chemistry(MOE) College of ChemistryNankai UniversityTianjin 300071China

Two-dimensional coordination polymers(CPs) have aroused tremendous interest as electrocatalysts because the catalytic performance could be fine-tuned by their well-designed coordination layers with highly accessible and active metal sites.However,it remains great challenge for CP-based catalysts to be utilized for electrocatalytic oxidation reactions due to their inefficient activities and low catalytic stabilities.Herein,we applied a mixed-metal strategy to fabricate two-dimensional Co_xNi_(1-x)-CPs with dual active sites for electrocatalytic water and urea oxidation.By metal ratio regulation in the twodimensional layer,an optimized Co_(2/3)Ni_(1/3)-CP exhibits a water oxidation performance with an overpotential of 325 mV at a current density of 10 mA cm^(-2) and a Tafel slope of 86 mV dec^(-1) in alkaline solution for oxygen evolution reaction.Importantly,a lower potential than that of commercial RuO_(2) is observed over20 mA cm^(-2).Co_(2/3)Ni_(1/3)-CP also displays a potential of 1.381 V at 10 mA cm^(-2) for urea oxidation reaction and a Tafel slope of 124 mV dec^(-1).This mixed-metal strategy to maximize synergistic effect of different metal centers may ultimately lead to promising electrocatalysts for small molecule oxidation reaction.

关键词： Coordination Polymers Electrocatalysis Oxygen Evolution reaction urea oxidation reaction

Asymmetric configuration activating lattice oxygen via weakening d-p orbital hybridization for efficient C/N separation in urea overall electrolysis

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Journal of Energy Chemistry 2024年第5期92卷 233-239页

作者： Chongchong Liu Peifang Wang Bin Hu Xiaoli Liu Rong Huang Gang Zhou Key Laboratory of Integrated Regulation and Resource Development on Shallow Lake of Ministry of Education College of EnvironmentHohai UniversityNanjing 210098JiangsuChina

urea oxidation reaction(UOR)is proposed as an exemplary half-reaction in renewable energy applications because of its low thermodynamical potential.However,challenges persist due to sluggish reaction kinetics and complex by-products separation.To this end,we introduce the lattice oxygen oxidation mechanism(LOM),propelling a novel UOR route using a modified CoFe layered double hydroxide(LDH)catalyst termed CFRO-7.Theoretical calculations and in-situ characterizations highlight the activated lattice oxygen(O_(L))within CFRO-7 as pivotal sites for UOR,optimizing the reaction pathway and accelerating the kinetics.For the urea overall electrolysis application,the LOM route only requires a low voltage of 1.54 V to offer a high current of 100 mA cm^(-2) for long-term utilization(>48 h).Importantly,the by-product NCO^(-)−is significantly suppressed,while the CO_(2)2/N_(2) separation is efficiently achieved.This work proposed a pioneering paradigm,invoking the LOM pathway in urea electrolysis to expedite reaction dynamics and enhance product selectivity.

关键词： Lattice oxygen urea oxidation reaction Overall electrolysis Products selectivity

一步法构筑双功能富含氧空位的花瓣状镍铝水滑石纳米薄片用于高性能超级电容器和尿素氧化

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Science China Materials 2022年第7期65卷 1805-1813页

作者：王宇辰刘瑶钰张曼刘碧莹赵志月严凯 Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology School of Environmental Science and EngineeringSun Yat-sen UniversityGuangzhou 510275China

镍基水滑石在能量存储(超级电容器)和转化(尿素氧化)领域是很有前景的电极材料.合理构建镍基水滑石的原子和电子结构对于实现其理想的电化学性能至关重要.本论文报道了一种简单、环境友好的一步法制备富含氧空位的花瓣状镍铝水滑石(NiAl... 详细信息

镍基水滑石在能量存储(超级电容器)和转化(尿素氧化)领域是很有前景的电极材料.合理构建镍基水滑石的原子和电子结构对于实现其理想的电化学性能至关重要.本论文报道了一种简单、环境友好的一步法制备富含氧空位的花瓣状镍铝水滑石(NiAl-LDHs)纳米薄片用于混合超级电容器和尿素氧化.性能最好的富氧空位NiAl-LDHs纳米薄片具有216.6 m^(2) g^(-1)的大比表面积和3.45×10^(-4)S cm^(-1)的高电导率,可在1 A g^(-1)的比电流下展示出2801 F g^(-1)(700 C g^(-1))的超高比电容.基于NiAl-LDHs//商业活性炭组装的混合超级电容器在400 W kg^(-1)比功率密度下可获得50.0 W h kg^(-1)的比能量,且循环10,000次后仍有91%的电容保持率.同时,NiAl-LDHs纳米薄片作为高效的尿素氧化电催化剂,在1 mol L^(-1)KOH和0.33 mol L^(-1)尿素中仅需1.42 V vs.可逆氢电极的氧化电位就可达到10 mA cm^(-2)的电流密度.由于NiAl-LDHs的纳米薄片结构暴露了更多的活性位点和丰富的氧空位,其电化学性能优于大部分报道的镍基水滑石.因此,本研究为多功能纳米能源材料的合理设计奠定了良好的基础.

关键词： layered double hydroxides nanosheets oxygen vacancy hybrid supercapacitor urea oxidation reaction

Controllable Ni/NiO interface engineering on N-doped carbon spheres for boosted alkaline water-to-hydrogen conversion by urea electrolysis

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Nano Research 2022年第8期15卷 7124-7133页

作者： Xiujuan Xu Xianbiao Hou Puyu Du Canhui Zhang Shucong Zhang Huanlei Wang Arafat Toghan Minghua Huang School of Materials Science and Engineering Ocean University of ChinaQingdao 266100China Chemistry Department Faculty of ScienceSouth Valley UniversityQena 83523Egypt Chemistry Department College of ScienceImam Mohammad Ibn Saud Islamic University(IMSIU)Riyadh 11623Saudi Arabia

Interface engineering has gradually attracted substantial research interest in constructing active bifunctional catalysts toward urea electrolysis.The fundamental understanding of the crystallinity transition of the components on both sides of the interface is extremely significant for realizing controllable construction of catalysts through interface engineering,but it still remains a challenge.Herein,the Ni/NiO heterogenous nanoparticles are successfully fabricated on the porous N-doped carbon spheres by a facile hydrothermal and subsequent pyrolysis strategy.And for the first time we show the experimental observation that the Ni/NiO interface can be fine-tuned via simply tailoring the heating rate during pyrolysis process,in which the crystalline/amorphous or crystalline/crystalline Ni/NiO heterostructure is deliberately constructed on the porous N-doped carbon spheres(named as CA-Ni/NiO@NCS or CC-Ni/NiO@NCS,respectively).By taking advantage of the unique porous architecture and the synergistic effect between crystalline Ni and amorphous NiO,the well-designed CA-Ni/NiO@NCS displays more remarkable urea oxidation reaction(UOR)and hydrogen evolution reaction(HER)activity than its crystalline/crystalline counterpart of CC-Ni/NiO@NCS.Particularly,the whole assembled two-electrode electrolytic cell using the elaborate CANi/NiO@NCS both as the anode and cathode can realize the current density of 10 mA·cm^(−2)at a super low voltage of 1.475 V(264 mV less than that of pure water electrolysis),as well as remarkable prolonged stability over 63 h.Besides,the H_(2)evolution driven by an AA battery and a commercial solar cell is also studied to enlighten practical applications for the future.

关键词： Ni/NiO controllable interface engineering urea oxidation reaction hydrogen evolution reaction urea electrolysis

H_(2)O_(2) treatment boosts activity of NiFe layered double hydroxide for electro-catalytic oxidation of urea

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Journal of Environmental Sciences 2023年第7期129卷 152-160页

作者： Jinshan Wei Jin Wang Xiaoming Sun College of Materials Science and Engineering Key Laboratory of Optoelectronic Devices and SystemsCollege of Physics and Optoelectronic EngineeringShenzhen UniversityShenzhen 518060China State Key Laboratory of Chemical Resource Engineering College of ChemistryBeijing University of Chemical TechnologyBeijing 100029China

urea oxidation reaction(UOR)provides a method for hydrogen production besides wastewater treatment,but the current limited catalytic activity has prevented the application.Herein,we develop a novel H_(2)O_(2) treatment strategy for tailoring the surface oxygen ligand of NiFe-layered double hydroxides(NiFe-LDH).The sample after H_(2)O_(2) treatment(NiFeOLDH)shows significant enhancement on UOR efficiency,with the potential of 1.37 V(RHE)to reach a current density of 10 mA/cm^(2).The boost is attributed to the richness adsorption O ligand on NiFeO-LDH as revealed by XPS and Raman analysis.DFT calculation indicates formation of two possible types of oxygen ligands:adsorbed oxygen on the surface and exposed from hydroxyl group,lowered the desorption energy of CO_(2) product,which lead to the lowered onset potential.This strategy is further extended to NiFe-LDH nano sheet on Ni foam to reach a higher current density of 440 mA/cm^(2) of UOR at 1.8 V(RHE).The facile surface O ligand manipulation is also expected to give chance to many other electro-catalytic oxidations.

关键词： NiFe-LDH urea oxidation reaction H_(2)O_(2)treatment Electro-catalysis Hydrogen production

Hierarchically wood-derived integrated electrode with tunable superhydrophilic/superaerophobic surface for efficient urea electrolysis

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Journal of Energy Chemistry 2023年第1期76卷 566-575,I0014页

作者： Yu Liao Songlin Deng Yan Qing Han Xu Cuihua Tian Yiqiang Wu College of Materials Science and Engineering Central South University of Forestry and TechnologyChangsha 410004HunanChina

Conferring surfaces with superhydrophilic/superaerophobic characteristics is desirable for synthesizing efficient gas reaction catalysts.However,complicated procedures,high costs,and poor interfaces hinder commercialization.Here,an integrated electrode with tunable wettability derived from a hierarchically porous wood scaffold was well designed for urea oxidation reaction(UOR).Interestingly,the outer surface of the wood lumen was optimized to the preferred wettability via stoichiometry to promote electrolyte permeation and gas escape.This catalyst exhibits outstanding activity and durability for UOR in alkaline media,requiring only a potential of 1.36 V(vs.RHE)to deliver 10 m A cm^(-2)and maintain its activity without significant decay for 60 h.These experiments and theoretical calculations demonstrate that the nickel(oxy)hydroxide layer formed through surface reconstruction of nickel nanoparticles improves the active sites and intrinsic activity.Moreover,the superwetting properties of the electrode promote mass transfer by guaranteeing substantial contact with the electrolyte and accelerating the separation of gaseous products during electrocatalysis.These findings provide the understanding needed to manipulate the surface wettability through rational design and fabrication of efficient electrocatalysts for gas-evolving processes.

关键词： Integrated electrode Wood scaffold Superhydrophilic/Superaerophobic surface urea oxidation reaction

Nested hollow architectures of nitrogen-doped carbon-decorated Fe,Co,Ni-based phosphides for boosting water and urea electrolysis

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Nano Research 2022年第3期15卷 1916-1925页

作者： Jie Zhang Shoushuang Huang Ping Ning Peijun Xin Zhiwen Chen Qing Wang Kajsa Uvdal Zhangjun Hu Shanghai Applied Radiation Institute School of Environmental and Chemical EngineeringShanghai UniversityShanghai 200444China Division of Molecular Surface Physics&Nanoscience Department of PhysicsChemistry and BiologyLinköping UniversityLinköping 58183Sweden

Tailoring the nanostructure/morphology and chemical composition is important to regulate the electronic configuration of electrocatalysts and thus enhance their performance for water and urea electrolysis.Herein,the nitrogen-doped carbon-decorated tricomponent metal phosphides of FeP4 nanotube@Ni-Co-P nanocage(NC-FNCP)with unique nested hollow architectures are fabricated by a self-sacrifice template strategy.Benefiting from the multi-component synergy,the modification of nitrogen-doped carbon,and the modulation of nested porous hollow morphology,NC-FNCP facilitates rapid electron/mass transport in water and urea electrolysis.NC-FNCP-based anode shows low potentials of 248 mV and 1.37 V(vs.reversible hydrogen electrode)to attain 10 mA/cm^(2) for oxygen evolution reaction(OER)and urea oxidation reaction(UOR),respectively.In addition,the overall urea electrolysis drives 10 mA/cm^(2) at a comparatively low voltage of 1.52 V(vs.RHE)that is 110 mV lower than that of overall water electrolysis,as well as exhibits excellent stability over 20 h.This work strategizes a multi-shell-structured electrocatalyst with multi-compositions and explores its applications in a sustainable combination of hydrogen production and sewage remediation.

关键词： tri-metal phosphides nested hollow nano-architecture oxygen evolution reaction urea oxidation reaction

Elucidating the promotion mechanism of the ternary cooperative heterostructure toward industrial-level urea oxidation catalysis

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Journal of Energy Chemistry 2023年第10期85卷 116-125,I0005页

作者： Xiujuan Xu Xiaotong Wei Liangliang Xu Minghua Huang Arafat Toghan School of Materials Science and Engineering Ocean University of ChinaQingdao 266100ShandongChina Department of Chemical and Biomolecular Engineering Korea Advanced Institute of Science and Technology(KAIST)291 Daehak-RoYuseong-GuDaejeon 34141Republic of Korea Chemistry Department College of ScienceImam Mohammad Ibn Saud Islamic University(IMSIU)Riyadh 11623Saudi Arabia Chemistry Department Faculty of ScienceSouth Valley UniversityQena 83523Egypt

From the perspective of electronic structure modulation,it is highly desirable to rationally design the active urea oxidation reaction(UOR)catalysts through interface engineering.The binary cooperative heterostructure systems have been shown significant enhancement for catalyzing UOR,but their performance still remains unsatisfactory for industrialization because of the unfavorable intermediate adsorption/desorption and deficient electron transfer channels.In response,taking the ternary cooperative Ni_5P_(4)/NiSe_(2)/Ni_(3)Se_(4) heterostructure as the proof-of-concept paradigm,a catalytic model is rationally put forward to elucidate the UOR promotion mechanism at the molecular level.The rod-like Ni_5P_(4)/NiSe_(2)/Ni_(3)Se_(4) nanoarrays with three-phase heterojunction are experimentally fabricated on Ni foam(named as Ni_5P_(4)/NiSe_(2)/Ni_(3)Se_(4)/NF)via simple two-step processes.The density functional theory calculations disclose that construction of Ni_5P_(4)/NiSe_(2)/Ni_(3)Se_(4) heterostructure model not only induce charge redistribution at the interfacial region for creating innumerable electron transfer channels,but also endow it with a moderate d-band center that could help to build a balance between adsorption and desorption of diverse UOR intermediates.Benefiting from the unique rod-like nanoarrays with large specific surface area and the optimized electronic structure,the well-designed Ni_5P_(4)/NiSe_(2)/Ni_(3)Se_(4)/NF could act as a robust catalyst for driving UOR at industrial-level current densities under tough environments,offering great potential for commercial applications.

关键词： urea oxidation reaction Ternary cooperative heterostructure Electronic structure Interface engineering