Mechanochemical-Assisted Synthesis of High-Entropy Metal Nitride via a Soft Urea Strategy

Jin, Tian; Sang, Xiahan; Unocic, Raymond R.; Kinch, Richard T.; Liu, Xiaofei; Hu, Jun; Liu, Honglai; Dai, Sheng

doi:10.1002/adma.201707512

Title: Mechanochemical-Assisted Synthesis of High-Entropy Metal Nitride via a Soft Urea Strategy

Journal Article · 24 April 2018 · Advanced Materials

DOI: https://doi.org/10.1002/adma.201707512 · OSTI ID:1462855

Jin, Tian ^[1]; Sang, Xiahan ^[2];

^[2]; Kinch, Richard T. ^[3]; Liu, Xiaofei ^[4]; Hu, Jun ^[4]; Liu, Honglai ^[4];

^[5]

East China Univ. of Science and Technology, Shanghai (China). State Key Lab. of Chemical Engineering. School of Chemistry and Molecular Engineering; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences
Univ. of Puerto Rico, San Juan, PR (United States). Dept. of Chemistry
East China Univ. of Science and Technology, Shanghai (China). State Key Lab. of Chemical Engineering. School of Chemistry and Molecular Engineering
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Science Division

Abstract Crystalline high‐entropy ceramics (CHC), a new class of solids that contain five or more elemental species, have attracted increasing interest because of their unique structure and potential applications. Up to now, only a couple of CHCs (e.g., high‐entropy metal oxides and diborides) have been successfully synthesized. Here, a new strategy for preparing high‐entropy metal nitride (HEMN‐1) is proposed via a soft urea method assisted by mechanochemical synthesis. The as‐prepared HEMN‐1 possesses five highly dispersed metal components, including V, Cr, Nb, Mo, Zr, and simultaneously exhibits an interesting cubic crystal structure of metal nitrides. By taking advantage of these unique features, HEMN‐1 can function as a promising candidate for supercapacitor applications. A specific capacitance of 78 F g ⁻¹ is achieved at a scan rate of 100 mV s ⁻¹ in 1 m KOH. In addition, such a facile synthetic strategy can be further extended to the fabrication of other types of HEMNs, paving the way for the synthesis of HEMNs with attractive properties for task‐specific applications.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); East China Univ. of Science and Technology, Shanghai (China); Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Basic Research Program of China; 111 Project of Ministry of Education of China

Grant/Contract Number:: AC05-00OR22725; 21507030; B08021

OSTI ID:: 1462855

Alternate ID(s):: OSTI ID: 1434377

Journal Information:: Advanced Materials, Vol. 30, Issue 23; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 312 works

Citation information provided by
Web of Science

References (43)

Colossal dielectric constant in high entropy oxides Bérardan, David; Franger, Sylvain; Dragoe, Diana physica status solidi (RRL) - Rapid Research Letters, Vol. 10, Issue 4 https://doi.org/10.1002/pssr.201600043	journal	March 2016
Entropy-stabilized oxides Rost, Christina M.; Sachet, Edward; Borman, Trent Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9485	journal	September 2015
Hydrogen-Evolution Catalysts Based on Non-Noble Metal Nickel-Molybdenum Nitride Nanosheets Chen, Wei-Fu; Sasaki, Kotaro; Ma, Chao Angewandte Chemie International Edition, Vol. 51, Issue 25 https://doi.org/10.1002/anie.201200699	journal	May 2012
Improving the Cycling Stability of Metal-Nitride Supercapacitor Electrodes with a Thin Carbon Shell Lu, Xihong; Liu, Tianyu; Zhai, Teng Advanced Energy Materials, Vol. 4, Issue 4 https://doi.org/10.1002/aenm.201300994	journal	October 2013
Synthesis and characterization of a binary noble metal nitride Gregoryanz, Eugene; Sanloup, Chrystele; Somayazulu, M. Nature Materials, Vol. 3, Issue 5 https://doi.org/10.1038/nmat1115	journal	April 2004
Ammonothermal Synthesis and Optical Properties of Ternary Nitride Semiconductors Mg-IV-N ₂ , Mn-IV-N ₂ and Li-IV ₂ -N ₃ (IV=Si, Ge) Häusler, Jonas; Niklaus, Robin; Minár, Ján Chemistry - A European Journal, Vol. 24, Issue 7 https://doi.org/10.1002/chem.201704973	journal	December 2017
Mesoporous Titanium Nitride-Enabled Highly Stable Lithium-Sulfur Batteries Cui, Zhiming; Zu, Chenxi; Zhou, Weidong Advanced Materials, Vol. 28, Issue 32 https://doi.org/10.1002/adma.201601382	journal	May 2016
Limitations and Improvement Strategies for Early-Transition-Metal Nitrides as Competitive Catalysts toward the Oxygen Reduction Reaction Luo, Junming; Tian, Xinlong; Zeng, Jianhuang ACS Catalysis, Vol. 6, Issue 9 https://doi.org/10.1021/acscatal.6b01618	journal	August 2016
Transition Metal Nitride Coated with Atomic Layers of Pt as a Low-Cost, Highly Stable Electrocatalyst for the Oxygen Reduction Reaction Tian, Xinlong; Luo, Junming; Nan, Haoxiong Journal of the American Chemical Society, Vol. 138, Issue 5 https://doi.org/10.1021/jacs.5b11364	journal	January 2016
Layered Lithium Iron Nitride: A Promising Anode Material for Li-Ion Batteries Rowsell, Jesse L. C.; Pralong, Valérie; Nazar, Linda F. Journal of the American Chemical Society, Vol. 123, Issue 35 https://doi.org/10.1021/ja0112745	journal	September 2001
All Metal Nitrides Solid-State Asymmetric Supercapacitors Zhu, Changrong; Yang, Peihua; Chao, Dongliang Advanced Materials, Vol. 27, Issue 31 https://doi.org/10.1002/adma.201501838	journal	July 2015
Transition-Metal Nitride Core@Noble-Metal Shell Nanoparticles as Highly CO Tolerant Catalysts Garg, Aaron; Milina, Maria; Ball, Madelyn Angewandte Chemie International Edition, Vol. 56, Issue 30 https://doi.org/10.1002/anie.201704632	journal	June 2017
Lithium transition metal nitrides with the modified morphology characteristics as advanced anode materials for lithium ion batteries Liu, Y.; Matsumura, T.; Imanishi, N. Electrochemistry Communications, Vol. 6, Issue 7 https://doi.org/10.1016/j.elecom.2004.04.021	journal	July 2004
Topotactic Transformation of Metal–Organic Frameworks to Graphene-Encapsulated Transition-Metal Nitrides as Efficient Fenton-like Catalysts Li, Xuning; Ao, Zhimin; Liu, Jiayi ACS Nano, Vol. 10, Issue 12 https://doi.org/10.1021/acsnano.6b07522	journal	November 2016
Understanding Co-Mo Catalyzed Ammonia Decomposition: Influence of Calcination Atmosphere and Identification of Active Phase Duan, Xuezhi; Ji, Jian; Yan, Xiaodong ChemCatChem, Vol. 8, Issue 5 https://doi.org/10.1002/cctc.201501275	journal	January 2016
Visible light-driven efficient overall water splitting using p-type metal-nitride nanowire arrays Kibria, M. G.; Chowdhury, F. A.; Zhao, S. Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms7797	journal	April 2015
A new class of high-entropy perovskite oxides Jiang, Sicong; Hu, Tao; Gild, Joshua Scripta Materialia, Vol. 142 https://doi.org/10.1016/j.scriptamat.2017.08.040	journal	January 2018
Solution Synthesis of Cu ₃ PdN Nanocrystals as Ternary Metal Nitride Electrocatalysts for the Oxygen Reduction Reaction Vaughn II, Dimitri D.; Araujo, Jose; Meduri, Praveen Chemistry of Materials, Vol. 26, Issue 21 https://doi.org/10.1021/cm5029723	journal	October 2014
Room temperature lithium superionic conductivity in high entropy oxides Bérardan, D.; Franger, S.; Meena, A. K. Journal of Materials Chemistry A, Vol. 4, Issue 24 https://doi.org/10.1039/C6TA03249D	journal	January 2016
Strategies Based on Nitride Materials Chemistry to Stabilize Li Metal Anode Zhu, Yizhou; He, Xingfeng; Mo, Yifei Advanced Science, Vol. 4, Issue 8 https://doi.org/10.1002/advs.201600517	journal	March 2017
High-Dielectric-Permittivity Layered Nitride CaTiN ₂ Li, Xiaohui; Wang, Xiaoming; Han, Yifeng Chemistry of Materials, Vol. 29, Issue 5 https://doi.org/10.1021/acs.chemmater.6b05226	journal	February 2017
One-step solid state reaction for the synthesis of ternary nitrides Co ₃ Mo ₃ N and Fe ₃ Mo ₃ N Wang, Liangbiao; Xian, Wanjun; Zhang, Kailong Inorganic Chemistry Frontiers, Vol. 4, Issue 12 https://doi.org/10.1039/C7QI00447H	journal	January 2017
Vanadium nitride as a novel thin film anode material for rechargeable lithium batteries Sun, Qian; Fu, Zheng-Wen Electrochimica Acta, Vol. 54, Issue 2 https://doi.org/10.1016/j.electacta.2008.07.057	journal	December 2008
Formation of amorphous aluminum tantalum nitride powders by mechanical alloying El‐Eskandarany, M. Sherif; Aoki, K.; Suzuki, K. Applied Physics Letters, Vol. 60, Issue 13 https://doi.org/10.1063/1.107251	journal	March 1992
H ₂ O ₂ -Assisted Synthesis of Porous N-Doped Graphene/Molybdenum Nitride Composites with Boosted Oxygen Reduction Reaction Liu, Xiaobo; Amiinu, Ibrahim Saana; Liu, Shaojun Advanced Materials Interfaces, Vol. 4, Issue 11 https://doi.org/10.1002/admi.201601227	journal	March 2017
High Rate Electrochemical Capacitors from Three-Dimensional Arrays of Vanadium Nitride Functionalized Carbon Nanotubes Zhang, Li; Holt, Chris M. B.; Luber, Erik J. The Journal of Physical Chemistry C, Vol. 115, Issue 49 https://doi.org/10.1021/jp205052f	journal	November 2011
Metal Nitride/Graphene Nanohybrids: General Synthesis and Multifunctional Titanium Nitride/Graphene Electrocatalyst Wen, Zhenhai; Cui, Shumao; Pu, Haihui Advanced Materials, Vol. 23, Issue 45, p. 5445-5450 https://doi.org/10.1002/adma.201102772	journal	October 2011
Recent advances in metal nitrides as high-performance electrode materials for energy storage devices Balogun, Muhammad-Sadeeq; Qiu, Weitao; Wang, Wang Journal of Materials Chemistry A, Vol. 3, Issue 4 https://doi.org/10.1039/C4TA05565A	journal	January 2015
Electronic properties of the binary noble metal nitride PtN: First-principles calculations Kanoun, M. B.; Goumri-Said, S. Physical Review B, Vol. 72, Issue 11 https://doi.org/10.1103/PhysRevB.72.113103	journal	September 2005
Cr[sub 1−x]Fe[sub x]N (0≦x≦1) Ternary Transition-Metal Nitrides as Anode Materials for Lithium-Ion Batteries Sun, Qian; Fu, Zheng-Wen Electrochemical and Solid-State Letters, Vol. 11, Issue 12 https://doi.org/10.1149/1.2988835	journal	January 2008
3D Porous Hierarchical Nickel-Molybdenum Nitrides Synthesized by RF Plasma as Highly Active and Stable Hydrogen-Evolution-Reaction Electrocatalysts Zhang, Yongqi; Ouyang, Bo; Xu, Jing Advanced Energy Materials, Vol. 6, Issue 11 https://doi.org/10.1002/aenm.201600221	journal	April 2016
Experimental Synthesis and Properties of Metastable CuNbN ₂ and Theoretical Extension to Other Ternary Copper Nitrides Zakutayev, Andriy; Allen, Amy J.; Zhang, Xiuwen Chemistry of Materials, Vol. 26, Issue 17 https://doi.org/10.1021/cm5018135	journal	August 2014
High-Entropy Metal Diborides: A New Class of High-Entropy Materials and a New Type of Ultrahigh Temperature Ceramics Gild, Joshua; Zhang, Yuanyao; Harrington, Tyler Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep37946	journal	November 2016
Metal Nitride and Metal Carbide Nanoparticles by a Soft Urea Pathway Giordano, Cristina; Erpen, Christian; Yao, Weitang Chemistry of Materials, Vol. 21, Issue 21 https://doi.org/10.1021/cm9018953	journal	November 2009
Supercapacitors based on composites of PANI with nanosheets of nitrogen-doped RGO, BC 1.5 N, MoS 2 and WS 2 Gopalakrishnan, K.; Sultan, S.; Govindaraj, A. Nano Energy, Vol. 12 https://doi.org/10.1016/j.nanoen.2014.12.005	journal	March 2015
Sponge-like Nickel and Nickel Nitride Structures for Catalytic Applications Shalom, Menny; Molinari, Valerio; Esposito, Davide Advanced Materials, Vol. 26, Issue 8 https://doi.org/10.1002/adma.201304288	journal	November 2013
Lithium molybdenum nitride (LiMoN2): the first metallic layered nitride Elder, S. H.; Doerrer, Linda H.; DiSalvo, F. J. Chemistry of Materials, Vol. 4, Issue 4 https://doi.org/10.1021/cm00022a033	journal	July 1992
Synthesis of Ternary Metal Nitride Nanoparticles Using Mesoporous Carbon Nitride as Reactive Template Fischer, Anna; Müller, Jens Oliver; Antonietti, Markus ACS Nano, Vol. 2, Issue 12, p. 2489-2496 https://doi.org/10.1021/nn800503a	journal	November 2008
Gallium Nitride Crystals: Novel Supercapacitor Electrode Materials Wang, Shouzhi; Zhang, Lei; Sun, Changlong Advanced Materials, Vol. 28, Issue 19 https://doi.org/10.1002/adma.201600725	journal	March 2016
Ultrafast-Charging Supercapacitors Based on Corn-Like Titanium Nitride Nanostructures Yang, Peihua; Chao, Dongliang; Zhu, Changrong Advanced Science, Vol. 3, Issue 6 https://doi.org/10.1002/advs.201500299	journal	October 2015
Hydrogen-Evolution Catalysts Based on Non-Noble Metal Nickel-Molybdenum Nitride Nanosheets Chen, Wei-Fu; Sasaki, Kotaro; Ma, Chao Angewandte Chemie, Vol. 124, Issue 25 https://doi.org/10.1002/ange.201200699	journal	May 2012
Transition‐Metal Nitride Core@Noble‐Metal Shell Nanoparticles as Highly CO Tolerant Catalysts Garg, Aaron; Milina, Maria; Ball, Madelyn Angewandte Chemie, Vol. 129, Issue 30 https://doi.org/10.1002/ange.201704632	journal	June 2017
Strategies Based on Nitride Materials Chemistry to Stabilize Li Metal Anode Zhu, Yizhou; He, Xingfeng; Mo, Yifei Digital Repository at the University of Maryland https://doi.org/10.13016/m2p26q396	text	January 2017

Cited By (21)

From Highly Purified Boron Nitride to Boron Nitride‐Based Heterostructures: An Inorganic Precursor‐Based Strategy Chen, Hao; Yang, Zhenzhen; Guo, Wei Advanced Functional Materials, Vol. 29, Issue 50 https://doi.org/10.1002/adfm.201906284	journal	September 2019
High‐Entropy Oxides: Fundamental Aspects and Electrochemical Properties Sarkar, Abhishek; Wang, Qingsong; Schiele, Alexander Advanced Materials, Vol. 31, Issue 26 https://doi.org/10.1002/adma.201806236	journal	March 2019
Entropy‐Maximized Synthesis of Multimetallic Nanoparticle Catalysts via a Ultrasonication‐Assisted Wet Chemistry Method under Ambient Conditions Liu, Miaomiao; Zhang, Zihao; Okejiri, Francis Advanced Materials Interfaces, Vol. 6, Issue 7 https://doi.org/10.1002/admi.201900015	journal	February 2019
Entropy‐Driven Mechanochemical Synthesis of Polymetallic Zeolitic Imidazolate Frameworks for CO ₂ Fixation Xu, Wei; Chen, Hao; Jie, Kecheng Angewandte Chemie, Vol. 131, Issue 15 https://doi.org/10.1002/ange.201900787	journal	March 2019
Entropy-Driven Mechanochemical Synthesis of Polymetallic Zeolitic Imidazolate Frameworks for CO ₂ Fixation Xu, Wei; Chen, Hao; Jie, Kecheng Angewandte Chemie International Edition, Vol. 58, Issue 15 https://doi.org/10.1002/anie.201900787	journal	March 2019
Gassing Behavior of High‐Entropy Oxide Anode and Oxyfluoride Cathode Probed Using Differential Electrochemical Mass Spectrometry Breitung, Ben; Wang, Qingsong; Schiele, Alexander Batteries & Supercaps, Vol. 3, Issue 4 https://doi.org/10.1002/batt.202000010	journal	April 2020
Mechanochemically Assisted Synthesis of Ruthenium Clusters Embedded in Mesoporous Carbon for an Efficient Hydrogen Evolution Reaction Liu, Xiaofei; Jin, Tian Leo; Hood, Zachary D. ChemElectroChem, Vol. 6, Issue 10 https://doi.org/10.1002/celc.201900618	journal	April 2019
Room‐Temperature Synthesis of High‐Entropy Perovskite Oxide Nanoparticle Catalysts through Ultrasonication‐Based Method Okejiri, Francis; Zhang, Zihao; Liu, Jixing ChemSusChem, Vol. 13, Issue 1 https://doi.org/10.1002/cssc.201902705	journal	November 2019
High-entropy ceramics Oses, Corey; Toher, Cormac; Curtarolo, Stefano Nature Reviews Materials, Vol. 5, Issue 4 https://doi.org/10.1038/s41578-019-0170-8	journal	February 2020
Morphology-maintaining synthesis of NbN and its catalytic performance in epoxidation Zhao, Tiaohao; Shen, Shanshan; Liu, Xiaohui Catalysis Science & Technology, Vol. 9, Issue 15 https://doi.org/10.1039/c9cy00890j	journal	January 2019
Multi-anionic and -cationic compounds: new high entropy materials for advanced Li-ion batteries Wang, Qingsong; Sarkar, Abhishek; Wang, Di Energy & Environmental Science, Vol. 12, Issue 8 https://doi.org/10.1039/c9ee00368a	journal	January 2019
Microwave-assisted depolymerization of various types of waste lignins over two-dimensional CuO/BCN catalysts Cao, Yang; Chen, Season S.; Tsang, Daniel C. W. Green Chemistry, Vol. 22, Issue 3 https://doi.org/10.1039/c9gc03553b	journal	January 2020
Low-temperature synthesis of small-sized high-entropy oxides for water oxidation Wang, Dongdong; Liu, Zhijuan; Du, Shiqian Journal of Materials Chemistry A, Vol. 7, Issue 42 https://doi.org/10.1039/c9ta08740k	journal	January 2019
First‐principles study, fabrication, and characterization of (Hf _0.2 Zr _0.2 Ta _0.2 Nb _0.2 Ti _0.2 )C high‐entropy ceramic Ye, Beilin; Wen, Tongqi; Huang, Kehan Journal of the American Ceramic Society, Vol. 102, Issue 7 https://doi.org/10.1111/jace.16295	journal	January 2019
One‐step synthesis of coral‐like high‐entropy metal carbide powders Ye, Beilin; Ning, Shanshan; Liu, Da Journal of the American Ceramic Society, Vol. 102, Issue 10 https://doi.org/10.1111/jace.16514	journal	April 2019
Two‐step synthesis process for high‐entropy diboride powders Feng, Lun; Fahrenholtz, William G.; Hilmas, Gregory E. Journal of the American Ceramic Society, Vol. 103, Issue 2 https://doi.org/10.1111/jace.16801	journal	September 2019
Gassing Behavior of High‐Entropy Oxide Anode and Oxyfluoride Cathode Probed Using Differential Electrochemical Mass Spectrometry Breitung, Ben; Wang, Qingsong; Schiele, Alexander Wiley https://doi.org/10.5445/ir/1000117436	text	January 2020
Multi-anionic and -cationic compounds: New high entropy materials for advanced Li-ion batteries Wang, Qingsong; Sarkar, Abhishek; Wang, Di Cambridge : Royal Society of Chemistry https://doi.org/10.15488/9843	other	January 2019
High-Entropy Oxides: Fundamental Aspects and Electrochemical Properties Sarkar, Abhishek; Wang, Qingsong; Schiele, Alexander Karlsruhe https://doi.org/10.5445/ir/1000093195	text	January 2019
Multi-anionic and -cationic compounds: new high entropy materials for advanced Li-ion batteries Wang, Qingsong; Sarkar, Abhishek; Wang, Di Cambridge : RSC https://doi.org/10.15488/10767	other	January 2019
Computationally aided, entropy-driven synthesis of highly efficient and durable multi-elemental alloy catalysts Yao, Yonggang; Liu, Zhenyu; Xie, Pengfei Science Advances, Vol. 6, Issue 11 https://doi.org/10.1126/sciadv.aaz0510	journal	March 2020