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Oxygen‑Coordinated Single Mn Sites for Efficient Electrocatalytic nitrate reduction to Ammonia

Nano-Micro Letters 2024年第1期16卷 147-159页

作者： Shengbo Zhang Yuankang Zha Yixing Ye Ke Li Yue Lin Lirong Zheng Guozhong Wang Yunxia Zhang Huajie Yin Tongfei Shi Haimin Zhang Laboratory of Materials Physics Centre for Environmental and Energy NanomaterialsAnhui Key Laboratory of Nanomaterials and NanotechnologyCAS Center for Excellence in NanoscienceInstitute of Solid State PhysicsHFIPSChinese Academy of SciencesHefei 230031People’s Republic of China University of Science and Technology of China Hefei 230026People’s Republic of China Key Laboratory of Agricultural Sensors Ministry of AgricultureSchool of Information and ComputerAnhui Agricultural UniversityHefei 230026People’s Republic of China Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026People’s Republic of China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of Sciences19B Yuquan RoadBeijing 100049People’s Republic of China

Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites with atomically dispersed oxygen(O)coordination on bacterial cellulose-converted graphitic carbon(Mn-O-C).Evidence of the atomically dispersed Mn-(O-C_(2))_(4)moieties embedding in the exposed basal plane of carbon surface is confirmed by X-ray absorption spectroscopy.As a result,the as-synthesized Mn-O-C catalyst exhibits superior NitRR activity with an NH_(3)yield rate(RNH_(3))of 1476.9±62.6μg h^(−1)cm^(−2)at−0.7 V(vs.reversible hydrogen electrode,RHE)and a faradaic efficiency(FE)of 89.0±3.8%at−0.5 V(vs.RHE)under ambient conditions.Further,when evaluated with a practical flow cell,Mn-O-C shows a high RNH_(3)of 3706.7±552.0μg h^(−1)cm^(−2)at a current density of 100 mA cm−2,2.5 times of that in the H cell.The in situ FT-IR and Raman spectroscopic studies combined with theoretical calculations indicate that the Mn-(O-C_(2))_(4)sites not only effectively inhibit the competitive hydrogen evolution reaction,but also greatly promote the adsorption and activation of nitrate(NO_(3)^(−)),thus boosting both the FE and selectivity of NH_(3)over Mn-(O-C_(2))_(4)sites.

关键词： Atomically dispersed Oxygen coordination nitrate reduction reaction In situ spectroscopic studies Hydrogen evolution reaction

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Screening of transition metal oxides for electrocatalytic nitrate reduction to ammonia at large currents

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Nano Research 2024年第5期17卷 3902-3910页

作者： Qiongfei Wu Weijie Zhu Dongxu Ma Chao Liang Zhoucheng Wang Hanfeng Liang State Key Laboratory of Physical Chemistry of Solid Surfaces Tan Kah Kee Innovation LaboratoryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China College of Chemical Engineering Tianjin UniversityTianjin 300072China

Electrochemical nitrate reduction reaction(NO_(3)RR)towards ammonia,as an emerging and appealing technology alternative to the energy-intensive Haber-Bosch process and inefficient nitrogen reduction reaction,has recently aroused wide concern and research.However,the current research of the NO_(3)RR towards ammonia lacks the overall performance comparison of various electrocatalysts.Given this,we here make a comparison of 12 common transition metal oxide catalysts for the NO_(3)RR under a high cathodic current density of 0.25 A·cm^(-2),wherein Co_(3)O_(4) catalyst displays the highest ammonia Faradaic efficiency(85.15%)and moderate activity(ca.-0.25 V vs.reversible hydrogen electrode).Other external factors,such as nitrate concentrations in the electrolyte and applied potential ranges,have also been specifically investigated for the NO_(3)RR.

关键词： nitrate reduction reaction ammonia production transition metal oxides Co_(3)O_(4)

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Electro-triggered Joule heating method to synthesize single-phase CuNi nano-alloy catalyst for efficient electrocatalytic nitrate reduction toward ammonia

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Nano Research 2023年第5期16卷 6632-6641页

作者： Zunjie Zhang Yang Liu Xiaozhi Su Ziwei Zhao Zhenkun Mo Chenyi Wang Yaling Zhao Ye Chen Shuyan Gao School of Chemistry and Chemical Engineering Henan Normal UniversityXinxiang 453007China School of Materials Science and Engineering Henan Normal UniversityXinxiang 453007China Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied PhysicsChinese Academy of SciencesShanghai 201204China

Electrochemical nitrate reduction reaction(NO_(3)RR)has great potential for ammonia(NH_(3))synthesis benefiting from its environmental friendliness and sustainability.Cu-based alloys with elemental diversity and adsorption tunability are widely used as electrocatalyst to lower the reaction overpotential for NO_(3)RR catalysis.However,phase separation commonly found in alloys leads to uneven distribution of elements,which limits the possibility of further optimizing the catalytic activity.Herein,an electrotriggered Joule heating method,possessing unique superiority of flash heating and cooling that lead to well-dispersed nanoparticles and uniform mixing of various elements,was adopted to synthesize a single-phase CuNi nano-alloy catalyst evenly dispersed on carbon fiber paper,CFP-Cu_(1)Ni_(1),which exhibited a more positive NO_(3)RR initial potential of 0.1 V versus reversible hydrogen electrode(vs.RHE)than that of pure copper nanoparticles at 10 mA·cm^(−2)in 0.5 mol·L^(−1)Na_(2)SO_(4)+0.1 mol·L^(−1)KNO_(3)solution.Importantly,CFP-Cu_(1)Ni_(1) presented high electrocatalytic activity with a Faradaic efficiency of 95.7%and NH_(3)yield rate of 180.58μmol·h^(−1)·cm^(−2)(2550μmol·h^(−1)·mg_(cat)^(−1))at−0.22 V vs.RHE.Theoretical calculations showed that alloying Cu with Ni into single-phase caused an upshift of its d-band center,which promoted the adsorption of NO_(3)−and weakened the adsorption of NH_(3).Moreover,the competitive adsorption of hydrogen ions was restrained until−0.24 V.This work offers a rational design concept with clear guidance for rapid synthesis of uniformly dispersed single-phase nano-alloy catalyst for efficient electrochemical NO_(3)RR toward ammonia.

关键词： ammonia nitrate reduction reaction CuNi nano-alloy single-phase adsorption energy

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High-throughput mechanistic study of highly selective hydrogen-bonded organic frameworks for electrochemical nitrate reduction to ammonia

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Journal of Energy Chemistry 2023年第12期87卷 408-415,I0011页

作者： Shuo Wang Yi Wang Yunfan Fu Tianfu Liu Guoxiong Wang State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina College of Energy University of Chinese Academy of SciencesBeijing 100039China

Hydrogen-bonded organic frameworks(HOFs),an emerging porous macrocyclic materials linked by hydrogen-bond,hold potential for gas separation and storage,sensors,optical,and electrocatalysts.Here,HOF-based electrocatalysts are rationally developed for nitrates reduction to ammonia,allowing not only to regulate wastewater pollution but also to accomplish carbon-neutral ammonia(NH_(3))synthesis.We preform high-throughput computational screening of thirty-six HOFs with various metals as active sites,denoted as HOF-M1,for nitrate reduction reaction(NO_(3)RR)toward NH_(3).We have implemented a hierarchical four-step screening strategy,and ultimately,HOF-Ti1 was selected based on its exceptional catalytic activity and selectivity in the NO_(3)RR process.Through additional analysis,we discovered that the d band center of the active metal sites serves as an effective parameter for designing and predicting the performance of HOFs in NO_(3)RR.This research not only showcases the immense potential of electrocatalysis in transforming NO_(3)RR into NH_(3)but also provides researchers with a compelling incentive to undertake further experimental investigations.

关键词： nitrate reduction reaction Ammonia synthesis Hydrogen-bonded organic frameworks High-throughput calculations Electrocatalysts

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Recent Advances of Cu-Based Materials for Electrochemical nitrate reduction to Ammonia

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Chinese Journal of Structural Chemistry 2022年第12期41卷 89-106页

作者： Tianlun Ren Youwei Sheng Mingzhen Wang Kaili Ren Lianlian Wang You Xu State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology College of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014P.R.China Department of Chemistry Baotou Teachers’CollegeBaotou 014030P.R.China

The pollution of nitrate in groundwater has become an environmental problem of general concern due to adverse human and ecological impacts. Treatment of nitrate-rich wastewater is of significance yet challenging for the conventional biological denitrification processes. Electrocatalytic nitrate-to-ammonia conversion emerges as one of the most promising avenues to remove environmentally harmful nitrate from various types of wastewaters while simultaneously producing value-added ammonia. Cu-based materials show great advantages in promoting selective electroreduction of nitrate to ammonia in terms of high nitrate conversion efficiency, ammonia selectivity and ammonia faradaic efficiency thanks to the 3d transition metal structure, low cost, high reserves, and excellent catalytic performance of Cu. In this review, we comprehensively overview the most recent advances in selective electrocatalytic nitrate-to-ammonia conversion using Cu-based materials. Various kinds of Cu-based materials including monometallic Cu catalysts, bimetallic Cu-based catalysts, Cu-based compounds, and Cu-based inorganicorganic hybrid materials and their derivatives are discussed in detail with emphasis on their structural and compositional features and functional mechanisms in promoting nitrate-to-ammonia conversion. Finally, a brief discussion on future directions, challenges and opportunities in this field is also provided.

关键词： copper nitrate reduction reaction ammonia synthesis electrocatalytic catalyst design

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Unveiling enzyme-mimetic active intermediate of a bioinspired oxo-MoS_(x) electrocatalyst for aqueous nitrate reduction

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Journal of Energy Chemistry 2021年第2期30卷 90-92,I0004页

作者： Yuting Wang Bin Zhang Department of Chemistry School of ScienceInstitute of Molecular PlusTianjin UniversityTianjin 300072China Tianjin Key Laboratory of Molecular Optoelectronic Sciences Tianjin UniversityTianjin 300072China

Excessive nitrate in groundwater has emerged as a serious environmental concern. The elevated nitrate concentration in drinking water causes a serious threat to public health on account of the possible transformation ... 详细信息

关键词： Active intermediates Electrocatalysis nitrate reduction reaction Enzyme mimic Neutral medium

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Boron-iron nanochains for selective electrocatalytic reduction of nitrate

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Chinese Chemical Letters 2021年第6期32卷 2073-2078页

作者： Fanfan Ni Yuanyuan Ma Junliang Chen Wei Luo Jianping Yang State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghai 201620China Institute of Functional Materials Donghua UniversityShanghai 201620China

The electrocatalysis of nitrate reduction reaction(NRR)has been considered to be a promising nitrate removal technology.Developing a highly effective iron-based electrocatalyst is an essential challenge for NRR.Herein,boron-iron nanochains(B-Fe NCs)as efficient NRR catalysts were prepared via a facile lowcost and scalable method.The Fe/B ratio of the B-Fe NCs-x can be elaborately adjusted to optimize the NRR catalytic performance.Due to the electron transfer from boron to metal,the metal-metal bonds are weakened and the electron density near the metal atom centers are rearranged,which are favor of the conversion from NO3-into N2.Moreover,the well-crosslinked chain-like architectures benefit the mass/electron transport to boost the exposure of abundant catalytic active sites.Laboratory experiments demonstrated that the optimized B-Fe NCs catalyst exhibits superior intrinsic electrocatalytic NRR activity of high nitrate conversion(~80%),ultrahigh nitrogen selectivity(~99%)and excellent long-term reactivity in the mixed electrolyte system(0.02 mol/L NaCl and 0.02 mol/L Na_(2)SO_(4)mixed electrolyte),and the electrocatalytic activity of the material shows poor performance at low chloride ion concentration(nitrate conversion of~61%and nitrogen selectivity of~57%in 0.005 mol/L NaCl and 0.035 mol/L Na_(2)SO_(4)mixed electrolyte).This study provides a broad application prospect for further exploring the highefficiency and low-cost iron-based functional nanostructures for electrocatalytic nitrate reduction.

关键词： Nanostructured iron Boron doping nitrate reduction reaction Electrocatalysis

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Grain Boundaries Engineering of Hollow Copper Nanoparticles Enables Highly Efficient Ammonia Electrosynthesis from nitrate

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CCS Chemistry 2022年第6期4卷 2053-2064页

作者： Qi Hu Yongjie Qin Xiaodeng Wang Hongju Zheng Keru Gao Hengpan Yang Peixin Zhang Minhua Shao Chuanxin He College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhenGuangdong 518060 Department of Chemical and Biological Engineering and Energy Institute The Hong Kong University of Science and TechnologyKowloonHong Kong 999077

Electrochemical nitrate reduction reaction(NO_(3)−RR)is an ideal route to produce ammonia(NH_(3))under ambient conditions.Although a markedly improved NH3 production rate has been achieved on the NO_(3)−RR compared with the nitrogen reduction reaction(NRR),the NH_(3) production rate of NO_(3)−RR is still well below the industrial Haber-Bosch route due to the lack of robust electrocatalysts for yielding high current densitieswith concurrently good suppression of hydrogen evolution reaction(HER).Herein,we describe an in situ electrochemical strategy for the synthesis of hollow carbon-coated Cu nanoparticles(NPs)(HSCu@C)with abundant grain boundaries(HSCu-AGB@C)for highly efficient NO_(3)−RR in both alkaline and neutral media.Impressively,in alkaline media,the HSCu-AGB@C can achieve a maximum NH3 Faradaic efficiency of 94.2% with an ultrahigh NH_(3) rate of 487.8 mmol g^(−1) cat h^(−1) at−0.2 V versus a reversible hydrogen electrode,more than 2.4-fold of the rate obtained in the Haber-Bosch.Both theoretic computations and experimental results uncover that the grain boundaries play the key to improve the NO_(3)−RR performance.Herein,the industrial-scale NH_(3) production ratemay open exciting opportunities for the practical electrosynthesis NH_(3) under ambient conditions.

关键词： grain boundaries hollow structures artificial ammonia production nitrate reduction reaction Haber-Bosch route

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调节Co_(3)O_(4)的价电子结构提高硝酸根还原制氨的催化活性

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Science China Materials 2023年第10期66卷 3901-3911页

作者：陈文达陈志达黄振城郑黎荣赵晓娟胡江涛曹慧群李永亮任祥忠欧阳晓平叶盛华颜学庆张黔玲刘剑洪 Graphene Composite Research Center College of Chemistry and Environmental EngineeringShenzhen UniversityShenzhen 518060China State Key Laboratory of Nuclear Physics and Technology and Key Laboratory of HEDP of the Ministry of EducationCAPTPeking UniversityBeijing 100871China Shenzhen Eigen-Equation Graphene Technology Co. Ltd.Shenzhen 518000China Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China School of Materials Science and Engineering Xiangtan UniversityXiangtan 411105China

通过硝酸根电化学还原反应将NO_(3)^(-)转化为NH_(3)是一种有前景的制氨和“绿氢”储存方案.Co_(3)O_(4)对于硝酸根还原析氨反应表现出较高的析氨法拉第效率和稳定性,有望成为理想的催化剂.然而,在Co_(3)O_(4)上发生硝酸根还原反应仍需... 详细信息

通过硝酸根电化学还原反应将NO_(3)^(-)转化为NH_(3)是一种有前景的制氨和“绿氢”储存方案.Co_(3)O_(4)对于硝酸根还原析氨反应表现出较高的析氨法拉第效率和稳定性,有望成为理想的催化剂.然而,在Co_(3)O_(4)上发生硝酸根还原反应仍需较高的过电位,从而阻碍了能量转换效率的提升.本文中,我们合成了Cu掺杂Co_(3)O_(4)多孔空心纳米球用作硝酸根还原析氨催化剂.Cu掺杂在保障析氨法拉第效率和稳定性的前提下大幅降低了反应所需的过电位,有效提高了析氨速率.实验和理论分析均表明,Cu掺杂使Co_(3)O_(4)的最高占据态能量上移,缩小了Co_(3)O_(4)的最高占据态与NO_(3)^(-)的最低未占据分子轨道之间的能垒,从而降低了电子从Co_(3)O_(4)向NO_(3)^(-)跃迁所需的过电位,赋予了Cu掺杂Co_(3)O_(4)多孔空心纳米球优异的硝酸根还原析氨电催化活性和耐久性.本研究为纳米材料的电化学性能调控研究提供了新的理论视角.

关键词： Co_(3)O_(4) nitrate reduction reaction ammonia frontier orbital

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纳米多孔Ru掺杂Cu协同调节反应中间体吸附与水分子解离促进电化学硝酸盐还原合成氨

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Science China Materials 2023年第11期66卷 4387-4395页

作者：崔玉环孙昌宁丁国鹏赵明葛欣张伟朱永福王智力蒋青 Key Laboratory of Automobile Materials Ministry of Educationand School of Materials Science and EngineeringJilin UniversityChangchun 130022China College of Chemistry and Environmental Science Hebei UniversityBaoding 071002China Key Laboratory of Mobile Materials MOE and School of Materials Science&Engineeringand Electron Microscopy CenterJilin UniversityChangchun 130012China

作为能源密集型Haber-Bosch工艺合成氨的一种新兴替代品,电化学硝酸盐还原反应(NO_(3)RR)在可持续合成氨和废水处理方面受到了关注.然而,由于缺乏有效的电催化剂,NO_(3)RR目前仍然面临氨产率低和选择性差的问题.本文报道了通过脱合金法... 详细信息

作为能源密集型Haber-Bosch工艺合成氨的一种新兴替代品,电化学硝酸盐还原反应(NO_(3)RR)在可持续合成氨和废水处理方面受到了关注.然而,由于缺乏有效的电催化剂,NO_(3)RR目前仍然面临氨产率低和选择性差的问题.本文报道了通过脱合金法制备的纳米双模式孔Ru掺杂Cu催化剂作为NO_(3)RR的电催化剂,在-0.2 V versus RHE的电位下表现出29.63±0.74 mg h^(-1)mg_(cat.)^(-1)的超高氨产率与97.3%±2.5%的法拉第效率,优于大多数报道的催化剂.密度泛函理论计算表明,在Cu中掺杂Ru可以优化中间体的吸附能,降低NO_(3)RR速控步骤的能垒.此外,Ru原子可以促进H2O的吸附/解离,为含N中间体氢化为NH_(3)提供活性氢.这项工作为NO_(3)RR等过程进行高性能催化剂的合理设计提供了新的途径.

关键词： nitrate reduction reaction ammonia synthesis na-noporous metal electrocatalysis density functional theory

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