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Overview of emerging catalytic materials for electrochemical green ammonia synthesis and process

Carbon Energy 2023年第12期5卷 31-82页

作者： Venkata Thulasivarma Chebrolu Daehee Jang Gokana Mohana Rani Chaeeun Lim Kijung Yong Won Bae Kim Department of Chemical Engineering Pohang University of Science and Technology(POSTECH)PohangGyeongbukSouth Korea Department of Biological Sciences and Bioengineering Inha UniversityIncheonRepublic of Korea

The concept of“green-ammonia-zero-carbon emission”is an emerging research topic in the global community and many countries driving toward decarbonizing a diversity of applications dependent on fossil fuels.In light of this,electrochemical nitrogen reduction reaction(ENRR)received great attention at ambient conditions.The low efficiency(%)and ammonia(NH_(3))production rates are two major challenges in making a sustainable future.Besides,hydrogen evolution reaction is another crucial factor for realizing this NH_(3)synthesis to meet the large-scale commercial demand.Herein,the(i)importance of NH_(3)as an energy carrier for the next future,(ii)discussion with ENRR theory and the fundamental mechanism,(iii)device configuration and types of electrolytic systems for NH_(3)synthesis including key metrics,(iv)then moving into rising electrocatalysts for ENRR such as single-atom catalysts(SACs),MXenes,and metal–organic frameworks that were scientifically summarized,and(v)finally,the current technical contests and future perceptions are discussed.Hence,this review aims to give insightful direction and a fresh motivation toward ENRR and the development of advanced electrocatalysts in terms of cost,efficiency,and technologically large scale for the synthesis of green NH_(3).

关键词： electrochemical ammonia synthesis hydrogen energy carrier metal-organic-frameworks MXenes single-atom-catalysts

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Recent advances and challenges of nitrogen/nitrate electro catalytic reduction to ammonia synthesis

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Frontiers in Energy 2024年第2期18卷 128-140页

作者： Junwen CAO Yikun HU Yun ZHENG Wenqiang ZHANG Bo YU Institute of Nuclear and New Energy Technology(INET) Collaborative Innovation Center of Advanced Nuclear Energy TechnologyTsinghua UniversityBeijing 100084China Department of Chemical Engineering University of WaterlooWaterlooOntario N2L 3G1Canada Institute of New Energy Materials and Engineering School of Materials Science and EngineeringFuzhou UniversityFuzhou 350108China

The Haber-Bosch process is the most widely used synthetic ammonia technology at present.Since its invention,it has provided an important guarantee for global food security.However,the traditional Haber-Bosch ammonia synthesis process consumes a lot of energy and causes serious environmental pollution.Under the serious pressure of energy and environment,a green,clean,and sustainable ammonia synthesis route is urgently needed.electrochemical synthesis of ammonia is a green and mild new method for preparing ammonia,which can directly convert nitrogen or nitrate into ammonia using electricity driven by solar,wind,or water energy,without greenhouse gas and toxic gas emissions.Herein,the basic mechanism of the nitrogen reduction reaction(NRR)to ammonia and nitrate reduction reaction(NO_(3)^(-))to ammonia were discussed.The representative approaches and major technologies,such as lithium mediated electrolysis and solid oxide electrolysis cell(SOEC)electrolysis for NRR,high activity catalyst and advanced electrochemical device fabrication for(NO_(3)^(-))RR and electrochemical ammonia synthesis were summarized.Based on the above discussion and analysis,the main challenges and development directions for electrochemical ammonia synthesis were further proposed.

关键词： electrochemical ammonia synthesis nitrogen nitrate nitrogen reduction reaction(NRR)to ammonia nitrate reduction reaction(NO_(3)^(-))RR

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One-step synthesis of N,P co-doped porous carbon electrocatalyst for highly efficient nitrogen fixation

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Nano Research 2022年第3期15卷 1779-1785页

作者： Sijia Zhao Jin Wang Peng Wang Shuang Wang Jinping Li College of Environmental Science and Engineering Taiyuan University of TechnologyJinzhong 030600China Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization Taiyuan University of TechnologyTaiyuan 030024China

Heteroatom-doped porous carbon has attracted many researchers’interests owing to their hierarchical porous and more active sites for nitrogen reduction reaction(NRR).However,the development of simple synthesis strategies to fabricate efficient catalyst is still remaining a challenge.In this work,a series of N,P co-doped porous carbon were prepared by one-step pyrolysis of zeolitic imidazolate framework(ZIF-8)and triphenylphosphine(TPP)under nitrogen atmosphere.The obtained catalyst by calcinating ZIF-8 and TPP with the mass ratio of 1:5 for three hours was named as PN-C-ZIF-8,which exhibited a high yield rate of ammonia(43.39μg·h^(–1)·mg^(–1)cat.)and Faraday efficiency(16.67%)in 0.05 M H2SO4 at–0.3 V.More importantly,the PN-C-ZIF-8 catalyst had superior selectivity that no hydrazine by-products were detected and long-term durability for 72 h.This study provides an idea for the convenient design and preparation of heteroatom doped carbon materials.

关键词： N P co-doped carbon-based catalyst electrochemical ammonia synthesis metal organic framework pyrolysis

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Crystal defect engineering of Bi_(2)Te_(3)nanosheets by Ce doping for efficient electrocatalytic nitrogen reduction

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Nano Research 2023年第5期16卷 6544-6551页

作者： Jianli Nan Yongqin Liu Daiyong Chao Youxing Fang Shaojun Dong College of Chemistry Jilin UniversityChangchun 130012China Changchun State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of Science and Technology of China Hefei 230026China

electrochemical nitrogen reduction reaction(NRR)is a promising method for the synthesis of ammonia(NH3).However,the electrochemical NRR process remains a great challenge in achieving a high NH3 yield rate and a high Faradaic efficiency(FE)due to the extremely strong N≡N bonds and the competing hydrogen evolution reaction(HER).Recently,bismuth telluride(Bi_(2)Te_(3))with two-dimensional layered structure has been reported as a promising catalyst for N_(2)fixation.Herein,to further enhance its NRR activity,a general doping strategy is developed to introduce and modulate the crystal defects of Bi_(2)Te_(3)nanosheets by adjusting the amount of Ce dopant(denoted as Ce_(x)-Bi_(2)Te_(3),where x represents the designed molar ratio of Ce/Bi).Meanwhile,the crystal defects can be designed and controlled by means of ion substitution and charge compensation.At−0.60 V versus the reversible hydrogen electrode(RHE),Ce_(0.3)-Bi_(2)Te_(3)exhibits a high NH_(3) yield(78.2μg·h^(−1)·mgcat^(−1)),a high FE(19.3%),excellent structural and electrochemical stability.Its outstanding catalytic activity is attributed to the tunable crystal defects by Ce doping.This work not only contributes to enhancing the NRR activity of Bi_(2)Te_(3)nanosheets,but also provides a reliable approach to prepare high-performance electrocatalysts by controlling the type and concentration of crystal defects for artificial N_(2)fixation.

关键词： electrochemical ammonia synthesis nitrogen reduction reaction (bismuth telluride)Bi_(2)Te_(3)nanosheets Ce doping crystal defects

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