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

《能源前沿（英文）》 doi: 10.1007/s11708-023-0908-2

摘要： 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 (NO3− RR) 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 NO3 − 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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Platinum on nitrogen doped graphene and tungsten carbide supports for ammonia electro-oxidation reaction

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 930-938 doi: 10.1007/s11705-021-2130-2

摘要： Ammonia electrooxidation reaction involving multistep electron-proton transfer is a significant reaction for fuel cells, hydrogen production and understanding nitrogen cycle. Platinum has been established as the best electrocatalyst for ammonia oxidation in aqueous alkaline media. In this study, Pt/nitrogen-doped graphene (NDG) and Pt/tungsten monocarbide (WC)/NDG are synthesized by a wet chemistry method and their ammonia oxidation activities are compared to commercial Pt/C. Pt/NDG exhibits a specific activity of 0.472 mA∙cm–2, which is 44% higher than commercial Pt/C, thus establishing NDG as a more effective support than carbon black. Moreover, it is demonstrated that WC as a support also impacts the activity with further 30% increase in comparison to NDG. Surface modification with Ir resulted in the best electrocatalytic activity with Pt-Ir/WC/NDG having almost thrice the current density of commercial Pt/C. This work adds insights regarding the role of NDG and WC as efficient supports along with significant impact of Ir surface modification.

关键词： Ammonia electro-oxidation reaction     electrocatalyst supports     platinum     nitrogen doped graphene     tungsten carbide    

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Multi-stage ammonia production for sorption selective catalytic reduction of NO

Chen ZHANG, Guoliang AN, Liwei WANG, Shaofei WU

《能源前沿（英文）》 2022年 第16卷 第5期   页码 840-851 doi: 10.1007/s11708-021-0797-1

摘要： Sorption selective catalytic reduction of nitrogen oxides (NOx) (sorption-SCR) has ever been proposed for replacing commercial urea selective catalytic reduction of NOx (urea-SCR), while only the single-stage sorption cycle is hitherto adopted for sorption-SCR. Herein, various multi-stage ammonia production cycles is built to solve the problem of relative high starting temperature with ammonia transfer (AT) unit and help detect the remaining ammonia in ammonia storage and delivery system (ASDS) with ammonia warning (AW) unit. Except for the single-stage ammonia production cycle with MnCl2, other sorption-SCR strategies all present overwhelming advantages over urea-SCR considering the much higher NOx conversion driven by the heat source lower than 100°C and better matching characteristics with low-temperature catalysts. Furthermore, the required mass of sorbent for each type of sorption-SCR is less than half of the mass of AdBlue for urea-SCR. Therefore, the multifunctional multi-stage sorption-SCR can realize compact and renewable ammonia storage and delivery with low thermal energy consumption and high NOx conversion, which brings a bright potential for efficient commercial de-NOx technology.

关键词： selective catalytic reduction (SCR)     nitrogen oxides (NOx)     ammonia     composite sorbent     chemisorption    

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Overlooked nitrogen-cycling microorganisms in biological wastewater treatment

《环境科学与工程前沿（英文）》 2021年 第15卷 第6期 doi: 10.1007/s11783-021-1426-2

摘要：

• AOA and comammox bacteria can be more abundant and active than AOB/NOB at WWTPs.

关键词： Ammonia oxidizing archaea (AOA)     Complete ammonia oxidizing (comammox) bacteria     Dissimilatory nitrate reduction to ammonium (DNRA) bacteria     Nitrate/nitrite-dependent anaerobic methane oxidizing (NOx-DAMO) microorganisms     Engineering application    

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Electrocatalytic reduction of NO to NH in ionic liquids by P-doped TiO nanotubes

《化学科学与工程前沿（英文）》 2023年 第17卷 第6期   页码 726-734 doi: 10.1007/s11705-022-2274-8

摘要： Designing advanced and cost-effective electrocatalytic system for nitric oxide (NO) reduction reaction (NORR) is vital for sustainable NH3 production and NO removal, yet it is a challenging task. Herein, it is shown that phosphorus (P)-doped titania (TiO2) nanotubes can be adopted as highly efficient catalyst for NORR. The catalyst demonstrates impressive performance in ionic liquid (IL)-based electrolyte with a remarkable high Faradaic efficiency of 89% and NH3 yield rate of 425 μg·h−1·mgcat.−1, being close to the best-reported results. Noteworthy, the obtained performance metrics are significantly larger than those for N2 reduction reaction. It also shows good durability with negligible activity decay even after 10 cycles. Theoretical simulations reveal that the introduction of P dopants tunes the electronic structure of Ti active sites, thereby enhancing the NO adsorption and facilitating the desorption of *NH3. Moreover, the utilization of IL further suppresses the competitive hydrogen evolution reaction. This study highlights the advantage of the catalyst−electrolyte engineering strategy for producing NH3 at a high efficiency and rate.

关键词： nitric oxide reduction reaction     electrcatalysis     ammonia production     phosphorus-doped titania    

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氮肥行业氨氮工程减排技术评估方法研究与应用

骆其金,谌建宇,王振兴,庞志华,叶万生

《中国工程科学》 2014年 第16卷 第8期   页码 88-92

摘要：

根据国家“十二五”氨氮总量控制和典型行业氨氮减排的技术需求，本文选择氮肥工业作为典型，研究共性的工程减排技术决策方法。针对目前国内环境技术评估以定性判断为主，缺乏可操作性强的综合评估方法的状况，提出了以费用效益分析为核心，层次分析+灰色关联度为次重因素的综合评估新方法，确定了该评估方法的数学模型和过程算法，并结合实例进行分析计算和验证。

关键词： 氨氮     总量控制     综合评估    

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Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reductionreaction

Lin LI, Cehuang FU, Shuiyun SHEN, Fangling JIANG, Guanghua WEI, Junliang ZHANG

《能源前沿（英文）》 2022年 第16卷 第5期   页码 812-821 doi: 10.1007/s11708-020-0669-0

摘要： The development of highly active nitrogen-doped carbon-based transition metal (M-N-C) compounds for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs) greatly helps reduce fuel cell cost, thus rapidly promoting their commercial applications. Among different M-N-C electrocatalysts, the series of Fe-N-C materials are highly favored because of their high ORR activity. However, there remains a debate on the effect of Fe, and rare investigations focus on the influence of Fe addition in the second heat treatment usually performed after acid leaching in the catalyst synthesis. It is thus very critical to explore the influences of Fe on the ORR electrocatalytic activity, which will, in turn, guide the design of Fe-N-C materials with enhanced performance. Herein, a series of Fe-N-C electrocatalysts are synthesize and the influence of Fe on the ORR activity are speculated both experimentally and theoretically. It is deduced that the active site lies in the structure of Fe-N , accompanied with the addition of appropriate Fe, and the number of active sites increases without the occurrence of agglomeration particles. Moreover, it is speculated that Fe plays an important role in stabilizing N as well as constituting active sites in the second pyrolyzing process.

关键词： oxygen reduction reaction     Fe-N-C     active sites     Fe addition     second heat treatment    

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IMPROVING NITROGEN SAFETY IN CHINA: NITROGEN FLOWS, POLLUTION AND CONTROL

《农业科学与工程前沿（英文）》 2022年 第9卷 第3期   页码 465-474 doi: 10.15302/J-FASE-2022454

摘要：

● It is necessary to address the N flows and their impacts on environment in China for sustainable N management.

关键词： barriers     future management     ammonia emissions     nitrogen input     water N pollution    

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ROOT EXUDATES FROM CANOLA EXHIBIT BIOLOGICAL NITRIFICATION INHIBITION AND ARE EFFECTIVE IN INHIBITING AMMONIA

《农业科学与工程前沿（英文）》 2022年 第9卷 第2期   页码 177-186 doi: 10.15302/J-FASE-2021421

摘要：

A range of plant species produce root exudates that inhibit ammonia-oxidizing microorganisms. This biological nitrification inhibition (BNI) capacity can decrease N loss and increase N uptake from the rhizosphere. This study sought evidence for the existence and magnitude of BNI capacity in canola ( Brassica napus). Seedlings of three canola cultivars, Brachiaria humidicola(BNI positive) and wheat ( Triticum aestivum) were grown in a hydroponic system. Root exudates were collected and their inhibition of the ammonia oxidizing bacterium, Nitrosospira multiformis, was tested. Subsequent pot experiments were used to test the inhibition of native nitrifying communities in soil. Root exudates from canola significantly reduced nitrification rates of both N. multiformis cultures and native soil microbial communities. The level of nitrification inhibition across the three cultivars was similar to the well-studied high-BNI species B. humidicola. BNI capacity of canola may have implications for the N dynamics in farming systems and the N uptake efficiency of crops in rotational farming systems. By reducing nitrification rates canola crops may decrease N losses, increase plant N uptake and encourage microbial N immobilization and subsequently increase the pool of organic N that is available for mineralization during the following cereal crops.

关键词： ammonia oxidizing microorganisms / biological nitrification inhibition / farming rotations / nitrogen cycling / nitrogen use efficiency    

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3O4 on HZSM-5 support: designing applicable catalysts for selective catalytic reductionof nitrogen oxides by ammonia

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1741-1754 doi: 10.1007/s11705-023-2332-x

摘要： Based on monolayer dispersion theory, Co3O4/ZSM-5 catalysts with different loadings have been prepared for selective catalytic reduction of nitrogen oxides by ammonia. Co3O4 can spontaneously disperse on HZSM-5 support with a monolayer dispersion threshold of 0.061 mmol 100 m–2, equaling to a weight percentage around 4.5%. It has been revealed that the quantities of surface active oxygen (O2–) and acid sites are crucial for the reaction, which can adsorb and activate NOx and NH3 reactants effectively. Below the monolayer dispersion threshold, Co3O4 is finely dispersed as sub-monolayers or monolayers and in an amorphous state, which is favorable to generate the two kinds of active sites, hence promoting the performance of ammonia selective catalytic reduction of nitrogen oxide. However, the formation of crystalline Co3O4 above the capacity is harmful to the reaction performance. 4% Co3O4/ZSM-5, the catalyst close to the monolayer dispersion capacity, possesses the most abundant active O2– species and acidic sites, thereby demonstrating the best reaction performance in all the samples. It is proposed the optimal Co3O4/ZSM-5 catalyst can be prepared by loading the capacity amount of Co3O4 onto HZSM-5 support.

关键词： Co3O4/ZSM-5     NOx-SCR by NH3     monolayer dispersion threshold effect     surface acid sites     surface active O2– anions    

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Simultaneous enhanced ammonia and nitrate removal from secondary effluent in constructed wetlands using

《环境科学与工程前沿（英文）》 2023年 第18卷 第4期 doi: 10.1007/s11783-024-1807-4

摘要：

● MnO2/PCL composite material (MPCM) enhances ammonia and nitrate removal in CWs.

关键词： Constructed wetland     Nitrogen removal     Manganese redox     Polycaprolactone     Nitrous oxide    

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Concurrent adsorption and reduction of chromium(VI) to chromium(III) using nitrogen-doped porous carbon

《环境科学与工程前沿（英文）》 2022年 第16卷 第5期 doi: 10.1007/s11783-021-1491-6

摘要：

• A high-efficiency N-doped porous carbon adsorbent for Cr(VI) was synthesized.

关键词： Chromium(VI)     Nitrogen-doped porous carbon     Adsorption     Reduction     Loofah sponge    

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Research progress and prospects of complete ammonia oxidizing bacteria in wastewater treatment

《环境科学与工程前沿（英文）》 2022年 第16卷 第9期 doi: 10.1007/s11783-022-1555-2

摘要：

• Comammox bacteria have unique physiological characteristics.

关键词： Complete ammonia oxidizing (comammox) bacteria     Nitrogen cycle     Physiological characteristics     Wastewater treatment    

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Selective reduction of NO by photo-SCR with ammonia in an annular fixed-film photoreactor

YiangChen CHOU, Young KU

《环境科学与工程前沿（英文）》 2012年 第6卷 第2期   页码 149-155 doi: 10.1007/s11783-010-0296-9

摘要： Gaseous NO was photocatalytically reduced at room temperature by photo-assisted selective catalytic reduction (photo-SCR) with ammonia over TiO in this study. NO reduction efficiency and N selectivity were determined from gases composition at the outlet stream of photoreactor. Effect of operating conditions, e.g. light intensity and inlet concentrations of ammonia and oxygen, on the NO reduction efficiency and N selectivity were discussed to determine the feasible operating condition for photocatalytic reduction of NO. Experimental results showed that selective catalytic reduction of NO with ammonia over TiO in the presence of oxygen was a spontaneous reaction in dark. The photoirradiation on the TiO surface caused remarkable photocatalytic reduction of NO to form N , NO , and N O under 254 nm UV illuminations, while almost 90% of N selectivity was achieved in this study. The ammonia and oxygen molecules played the roles of reductant and oxidant for NO reduction and active sites regeneration, respectively. The reduction of NO was found to be increased with the increase of inlet ammonia and oxygen concentrations until specific concentrations because of the limited active sites on the surface of TiO . The kinetic model proposed in this study can be used to reasonably describe the reaction mechanism of photo-SCR.

关键词： photo-SCR     photocatalysis     NO reduction     Eley-Rideal model    

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Design guidelines for urea hydrolysers for ammonia demand of the SCR DENOX project in coal-fired power

Peng ZHENG, Xuan YAO, Wei ZHENG

《能源前沿（英文）》 2013年 第7卷 第1期   页码 127-132 doi: 10.1007/s11708-012-0225-7

摘要： Ammonia is highly volatile and will present substantial environmental and operation hazards when leaking into the air. However, ammonia is the most common reactant in the DENOX project to eliminate NO in the flue gas. The storage and transportation of liquid ammonia has always been a dilemma of the power plant. Urea is a perfect substitute source for ammonia in the plant. Urea hydrolysis technology can easily convert urea into ammonia with low expense. Presently, there is still no self-depended mature urea hydrolysis technology for the DENOX project in China; therefore, this paper proposes several guidelines to design the urea hydrolyser by theoretical analysis. Based on theoretical analysis, a simulation model is built to simulate the chemical reaction in the urea hydrolyser and is validated by the operational data of the commercial hydrolyser revealed in the literature. This paper endeavors to propose suggestions and guidelines to develop domestically urea hydrolysers in China.

关键词： urea     hydrolyser     ammonia     selective catalytic reduction (SCR)    

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标题 作者 时间 类型 操作

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

期刊论文

Platinum on nitrogen doped graphene and tungsten carbide supports for ammonia electro-oxidation reaction

期刊论文

Multi-stage ammonia production for sorption selective catalytic reduction of NO

Chen ZHANG, Guoliang AN, Liwei WANG, Shaofei WU

期刊论文

Overlooked nitrogen-cycling microorganisms in biological wastewater treatment

期刊论文

Electrocatalytic reduction of NO to NH in ionic liquids by P-doped TiO nanotubes

期刊论文

氮肥行业氨氮工程减排技术评估方法研究与应用

骆其金,谌建宇,王振兴,庞志华,叶万生

期刊论文

Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reductionreaction

Lin LI, Cehuang FU, Shuiyun SHEN, Fangling JIANG, Guanghua WEI, Junliang ZHANG

期刊论文

IMPROVING NITROGEN SAFETY IN CHINA: NITROGEN FLOWS, POLLUTION AND CONTROL

期刊论文

ROOT EXUDATES FROM CANOLA EXHIBIT BIOLOGICAL NITRIFICATION INHIBITION AND ARE EFFECTIVE IN INHIBITING AMMONIA

期刊论文

3O4 on HZSM-5 support: designing applicable catalysts for selective catalytic reductionof nitrogen oxides by ammonia

期刊论文

Simultaneous enhanced ammonia and nitrate removal from secondary effluent in constructed wetlands using

期刊论文

Concurrent adsorption and reduction of chromium(VI) to chromium(III) using nitrogen-doped porous carbon

期刊论文

Research progress and prospects of complete ammonia oxidizing bacteria in wastewater treatment

期刊论文

Selective reduction of NO by photo-SCR with ammonia in an annular fixed-film photoreactor

YiangChen CHOU, Young KU

期刊论文

Design guidelines for urea hydrolysers for ammonia demand of the SCR DENOX project in coal-fired power

Peng ZHENG, Xuan YAO, Wei ZHENG

期刊论文