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Research progress in high-temperature SCR denitration: from catalyst innovations to reaction mechanism exploration
WANG Yu;TANG Tianfa;ZHOU Qinyu;XU Lu;TANG Changjin;[Objective]To meet the strict pollution control requirement for treating flue gas in scenarios like gas turbines and coalbed methane power generation,the development of efficient SCR catalysts that can perform well under high temperatures (>500℃) becomes very urgent,mainly due to the evident activity loss caused by serious sintering and aggravated NH3 over-oxidation for the commercial catalysts of V2O5-TiO2.[Methods]A systematic review was conducted on two categories of high-temperature catalysts:zeolite-based and metal oxide-based.Preparation methods performance optimization strategies,and reaction mechanisms were analyzed.In-situ FTIR and poisoning resistance experiments were employed to investigate NH3-SCR pathways,hydrothermal stability,and resistance to sulfur/alkal metal poisoning under high temperatures.[Results]For zeolite-based catalysts,Fe/SSZ-13 and Cu-SSZ-13 exhibited outstanding performance due to isolated metal sites and synergistic acid-redox properties.Among oxide-based catalysts,WO3-FeO?and sulfated CeO2 achieved high efficiency by enhancing surface acidity,oxygen vacancies,and suppressing NH3 oxidation.Poisoning resistance studies revealed that ZrO2 doping improved sulfur tolerance,while Ce doping mitigated alkali metal poisoning.[Conclusion]Zeolite-and oxide-based catalysts demonstrate potential for high temperature denitration,yet require further optimization in anti-deactivation mechanisms.Future research should focus on elucidating microstructural degradation under high temperatures;dynamic sulfur salt behavior and alkali meta trapping strategies;multi-pollutant synergistic control and practical adaptation of monolithic catalysts.
Research and prospect of Bi-based catalyst for electroreduction of CO2 to formic acid under the background of double carbon
CAO Yuanbo;YANG Tao;CHEN Bing;ZHANG Hong;YANG Liming;ZHOU Bing;ZHENG Yanhui;HOU Xinmei;[Objective] In order to improve the efficiency of electrocatalytic reduction of CO2 emitted by the thermal power industry to formic acid(HCOOH) and reduce the emission level of CO2 in the atmospheric environment,[Methods] In this paper, the improvement direction of high-efficiency Bi-based catalysts was proposed by analyzing the pathways of electrochemical carbon dioxide reduction reaction(ECO2RR) and the electrocatalytic effects of Bi metalbased catalysts under different control strategies. [Results] Studies have shown that Bi-based catalysts can achieve a Faraday efficiency greater than 85% when the stable operation time in the electrolytic cell is greater than 100 h. Bibased ECO2RR catalysts can be regulated from four aspects : surface morphology design, surface modification, defect engineering and component regulation. The surface morphology design can provide more active sites, but it cannot meet the practical application requirements of commercial scale HCOOH production. Surface modification can have beneficial effects on selectivity and activity, but there are problems such as stability, cost and mechanism. Defect engineering can optimize the charge transfer in the reaction and the bonding strength of the intermediate, but the controllability and mechanism of defects need to be studied. Component regulation can be carried out from three aspects: Element doping, alloying, and heterostructure construction. It is an important way to optimize the Bi-based ECO2RR reaction, but it also needs to supplement the test and calculation that are more in line with industrial development. [Conclusion] Bi-based catalysts have outstanding potential in the industrial application of electroreduction of CO2 to HCOOH. More in-depth improvement and mechanism research can accelerate the industrialization of CO2-derived chemicals.
Research on the mechanism of methane reforming based on Ni-Na2ZrO3adsorption-catalytic bifunctional material
SUN Chao;XIE Huaqing;XU Haijian;ZHANG Shu;LIU Kun;[Objective]This study aims to elucidate the microscopic reaction mechanism of Ni-Na2ZrO3 bifunctional material in sorption-enhanced methane steam reforming,addressing the challenges of high energy consumption in CO2separation and severe carbon deposition in traditional methane reforming.By optimizing material design through theoretical simulations,it provides a scientific basis for developing efficient and low-energy bifunctional materials,promoting the large-scale application of hydrogen energy and achieving carbon neutrality goals.[Methods]Based on density functional theory,a Ni-Na2ZrO3 surface model was constructed to systematically analyze the adsorption energies and competitive adsorption characteristics of 21 adsorbates (including CHx,CHxOH,CO,CO2,etc.) at different adsorption sites.Transition state calculations were performed to determine the energy barriers of 34 elementary reactions,investigating the kinetic pathways of methane dissociation,intermediate conversion,and CO2 formation.Key steps and rate-limiting stages of carbon conversion were identified by integrating surface energy,adsorption energy,and reaction barrier data.Furthermore,the CO2 adsorption-desorption performance of Na2ZrO3 and Ni-Na2ZrO3 was compared to evaluate the impact of Ni doping on material regenerability.[Results]The results indicate that the absolute adsorption energy of CH?and CHxOH increases significantly with dehydrogenation,C adsorption energy:-8.69 eV vs.CH4:-0.45 eV,demonstrating enhanced interaction between dehydrogenated species and the surface.Among the products,H2 exhibits weak adsorption,facilitating its desorption,while CO2 remains stably adsorbed,enabling in-situ separation.The optimal methane dissociation pathway follows direct dehydrogenation (CH4→CH3→CH2→CH),with CH3→CH2+H as the ratelimiting step (energy barrier:1.59 eV).The intermediate CH generates CO via the CHOH pathway (barrier:1.38 eV),and CO is further oxidized to CO2 with O atoms provided by OH dissociation.Ni doping significantly enhances regenerability:the adsorption energy of ZrO2 on Ni-Na2CO3 increases to-9.74 eV,and the CO2 desorption barrier decreases from 4.90 eV to 2.05 e V,drastically reducing regeneration energy consumption.[Conclusion]The Ni-Na2ZrO3 bifunctional material demonstrates high carbon conversion efficiency and exceptional cyclic stability in SESMR.The optimal reaction pathway(CH4→CO2) is achieved through coupling direct dehydrogenation and the CHOH pathway,with clearly defined rate-limiting steps.Ni incorporation strengthens the adsorption interface and lowers desorption barriers,significantly improving CO2capture and material regeneration.This study establishes a theoretical framework for designing dual-function materials with high catalytic activity and regenerability,offering critical insights for advancing low-energy hydrogen production and carbon capture technologies.
Research progress of manganese-based low-temperature SCR denitrification catalysts
LI Fangxiao;LIU Jinhao;WANG Ruiting;MA Jingwen;[Objective]Vanadium-based catalysts face challenges such as poor low-temperature activity and susceptibility to poisoning in selective catalytic reduction (SCR) technology,while manganese-based catalysts have emerged as a research hotspot due to their excellent low-temperature performance.This paper systematically reviews the types,structures,and anti-poisoning strategies of manganese-based catalysts to promote their industrial application in denitrification.[Methods]By summarizing recent studies,manganese-based catalysts are categorized into multi-meta manganese oxides and supported catalysts (metal oxides,carbon-based materials,molecular sieves).Anti-poisoning strategies include:1) Metal doping (e.g.,Fe,Ce,Ni) to optimize redox properties;2) Carrier optimization (e.g.,TiO2carbon composites) to enhance dispersion and stability;3) Morphological design (e.g.,nanorods,core-shell structures to inhibit sulfate deposition.[Results]Metal doping significantly increases the Mn4+ratio,e.g.,Fe-Mn/TiO2 achieves97.7%NO conversion at 150°C.Carrier optimization,such as TiO2-supported Mn catalysts,maintains stability under H2O for 10 days.Morphological modifications,like MnOx/CeO2 nanorods,show no activity loss after 1000 hours in 572 mg/m SO2.Bimetallic doping (e.g.,Fe:Co molar ratio 2:4) improves sulfur resistance by 30%.[Conclusion]Manganese-based catalysts exhibit enhanced low-temperature activity and anti-poisoning performance through multi-component doping carrier synergy,and structural design.However,challenges such as long-term stability,impacts of multi-pollutants (e.g.heavy metals,VOCs),and cost require further investigation.Future research should focus on eco-friendly modifications and in-situ mechanistic studies to facilitate industrial adoption.
Preparation of plant-based activated carbon and its application in the field of power generation
WEN Xiaojin;MA Dafu;LI Wangfan;WU Helai;DING Xian;[Objective]The aim of this paper is to systematically sort out the preparation technology of plant-based activated carbon,analyse the influence of key process parameters such as carbonisation,activation and modification on its performance,and assess its application potential through economic analysis in order to promote its large-scale application in the field of power generation.[Methods]Focusing on the preparation process of plant-based activated carbon,we systematically compare the effects of different carbonisation methods,such as direct carbonisation hydrothermal carbonisation and microwave carbonisation,and different activation methods,such as physical,chemical physicochemical,microwave-assisted chemical and catalytic activation,on the pore structure,specific surface area and adsorption performance of the activated carbon;we also explore the regulation mechanism of surface functional groups and selectivity by physical,chemical and metal-loaded modification methods;we elaborate its specific application scenarios based on the needs of the power generation field.The study also discusses the modulation mechanism o surface functional groups and selectivity by physical,chemical and metal loading modification methods.[Results]The study shows that (1) direct carbonisation is faster than hydrothermal carbonisation,but with higher energy consumption,but hydrothermal carbonisation has lower energy consumption and wider characteristics of activated carbon,so it has a wider application;(2) physical activation can effectively reduce the activation temperature by using O2 as an activator.Chemical activation and physicochemical activation mainly regulate the surface properties and pore size distribution of activated carbon,respectively;microwave-assisted and catalytic activation can improve the activation reaction process to a certain extent;microwave-assisted activation can reduce the surface acidity of activated carbon,and catalytic activation can regulate the pore size distribution of activated carbon to a certain range according to the difference in the sizes of the metal-oxide catalyst particles;(3) the economic analysis shows that combining the gasification with the gasification can reduce the energy consumption.heating/power generation can reduce energy consumption,and the production cost of plant-based activated carbon can be reduced by 30%～50%compared with coal-based,and it's more economical (4) in the field of power generation,plant-based activated carbon can adsorb dioxin with an efficiency of more than 99%and can be desulphurised and denitrified at the same time;as a catalyst carrier for electrolysis of water,it can increase the rate of hydrogen production by 45%;and as a supercapacitor material,it can achieve an energy density of 136.6 W·h/kg,which is significantly better than traditional materials.[Conclusion]Plant-based activated carbon,with its high specific surface area,adjustable pore structure and rich surface functional groups,shows a broad application prospect in the fields of flue gas treatment,electrocatalysis and energy storage in power plants.In the future,it is necessary to further optimise the energy efficiency and economy of the preparation process,and to promote its technical large-scale development,so as to help the low-carbon development of the power industry.
Process performance study of ZnZrOx solid solution catalysts in the hydrogenation of carbon dioxide to methanol
WANG Muhan;ZHOU Yu;SHEN Kai;ZHANG Yaping;[Objective]Methanol, a key industrial chemical, can be synthesized via CO2 hydrogenation using renewable hydrogen, serving as an effective pathway toward carbon neutrality. This study aims to optimize the process conditions of ZnZrO? solid solution catalysts for CO2 hydrogenation to methanol, focusing on temperature, pressure, space velocity,H2/CO2 ratio, and the role of a hydrophobic agent, providing guidance for industrial applications. [Methods]ZnZrO ?catalysts were prepared via ball milling. Catalytic performance was evaluated in a fixed-bed reactor under varied conditions(temperature, pressure, space velocity, H2/CO2molar ratio). In situ diffuse reflectance infrared Fourier transform spectroscopy was employed to analyze reaction intermediates. Additionally, hydrophobic polydivinylbenzene was physically mixed with the catalyst to enhance water removal and methanol synthesis. [Results]Optimal conditions were determined as 320 °C, 5 MPa, and 24 000 mL/(gcat·h), achieving a CO2 conversion of 5.1%, methanol selectivity of72.2%, and maximum methanol yield. Increasing the H2/CO2 ratio from 3 to 9 improved CO2 conversion to 12.9% and methanol yield by 145.8%, with DRIFTS revealing accelerated formate intermediate formation. Introducing PDVB(mass ratio 1: 1) facilitated water removal, boosting methanol yield to 414.0 mg/(gcat·h) at 320 ° C. [Conclusions]The ZnZrO?catalyst exhibited high efficiency under optimized conditions, while PDVB integration further enhanced methanol productivity. This study offers valuable insights for industrial CO2 utilization and catalyst design in sustainable chemical synthesis.
Research on the characteristics and recycling technology of regenerated wastewater from denitrification catalyst
YANG Jianhui;LI Han;CHENG Xi;ZHOU Mei;ZHAO Jianxin;XU Guanghui;YU Runwei;[Objective] To elucidate the indicators of harmful metal ions in wastewater discharge and reuse, and to provide superior solutions for the recycling of wastewater from the regeneration of waste catalysts, this paper systematically studied the ultrasonic wastewater and acid washing wastewater generated during the regeneration process of waste denitration catalysts at a coal-fired power plant. [Methods] By continuously washing the waste catalyst module, the main characteristics and component features of the ultrasonic and acid washing wastewater produced during the regeneration process of waste catalysts were identified. [Results] After cleaning 25 catalyst modules, the concentrations of various metal ions in the cleaning solution reach adsorption-dissolution equilibrium at the solid-liquid interface. Cleaning efficacy noticeably decreases after cleaning over 80 catalyst modules, also contaminating catalysts with minor chemical poisoning. The impregnation method was employed to simulate the poisoning of new denitration catalysts, and the study explored the accumulation patterns of metal ions in wastewater and the adsorption rules of harmful metal ions on the surface of the catalyst, investigating the correlation between the content of metal ions adsorbed on the surface of the poisoned catalyst and the denitrification efficiency of the catalyst. In the solution, when the Fe ion concentration exceeds 1.0%, the catalyst's denitrification efficiency decreases to around 50% and remains almost unchanged. When the Cr ion concentration in the solution increases from 1.0% to 3.0%, the catalyst's denitrification efficiency gradually increases and then stabilizes. [Conclusion] Therefore, the impact of Fe and Cr elements in the regenerated wastewater on the catalyst's denitrification efficiency is almost negligible. When the concentrations of K, Na, Ca, Pb, Hg, and As respectively reach 0.700%, 0.500%-0.600%, 0.100%, 0.045%, 0.400%-0.500% and 0.020%, it becomes necessary to promptly desalinate or treat ultrasonic and acid-washing wastewater to ensure effective regeneration and activation of the catalysts.
Key issues and application challenges of electrochemical energy storage materials and devices under extreme conditions
LI Bosen;HU Jinqiao;YU Binkai;LI Ye;WANG Hui;ZHANG Shengli;CHEN Mingzhe;【Objective】 Under the background of the transformation of energy structure to decarbonisation,electrochemical energy storage technology has become a key support to promote the large-scale application of renewable energy by virtue of its high energy conversion efficiency. However, the performance degradation of energy storage devices in extreme environments has significantly limited their practical application potential. In order to systematically study the key impact mechanisms of extreme environments on electrochemical energy storage materials and devices, we propose targeted optimisation strategies to enhance the adaptability of energy storage devices to extreme environments. [Methods] This paper systematically investigates the key influence mechanisms of extreme environments on electrochemical energy storage materials and devices, and focuses on four optimisation strategies by analysing the mechanism of four types of extreme environments: low-temperature electrolyte modification, hightemperature-resistant electrode material development, biomimetic interfacial buffer structure construction, and salt corrosion-resistant material research and development. [Results] The modification strategy significantly improves the adaptability of energy storage devices to extreme environments: 1) low-temperature electrolyte modification, based on deep eutectic solvent and high concentration of lithium salt electrolyte, achieving ionic conductivity of 4.8 mS/cm at-50 ℃, with a cycling efficiency of 92%; 2) development of high-temperature-resistant materials, the NASICON-type composite cathode has a capacity retention rate of 91.3% after cycling for 500 times at 80 ℃.(3) interface engineering optimization, bionic gradient buffer layer design makes the electrode under 15 MPa mechanical stress interface delamination rate reduced by 67%, the cycle life is extended by 3 times;(4) anti-salt corrosion materials, hydrophobic two-dimensional new material(MXene)/polymer composite coatings in the high-salinity environment will be the corrosion rate suppressed to 0.02 mm/a, the electrochemical efficiency of the attenuation rate decreased by 58%. [Conclusion] Future research should focus on key materials such as zero-strain alloy electrodes and biomimetic ion-channel electrolytes, and build a multi-scale failure analysis model and standard evaluation system. Through interdisciplinary integration, electrochemical energy storage technology will be promoted from the laboratory to the extreme environments such as deep sea and deep space for large-scale application, supporting the global energy transition.
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Introduction
Electric Power Technology and Environmental Protection
Bimonthly issued
CN 32-1808/X
ISSN 1674-8069
Governed by:
China Energy Investment Group Co., Ltd.
Sponsored by:
China Energy Group Science and Technology Research Institute Co., Ltd.
Academic support：
State Key Laboratory of Low-carbon Smart Coal-fired PowerGeneration and Ultra-clean Emission
Columns:
Thermal Energy Engineering, Clean Power Generation, New Energy Generation, Integrated Power Generation.
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