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Multi-objective optimization of methane production system from biomass through anaerobic digestion

Chinese Journal of Chemical engineering 2018年第10期26卷 2084-2092页

作者： Weijun Li Jakob Kj?bsted Huusom Zhimao Zhou Yi Nie Yajing Xu Xiangping Zhang Beijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Sino-Danish Center for Education and Research University of Chinese Academy of Sciences Department of Chemical & Biochemical Engineering Technical University of Denmark

This work addressed the multi-objective optimization of a biogas production system considering both environmental and economic criteria. A mixed integer non-linear programming(MINLP) model was established and solved with non-dominated sorting genetic algorithm Ⅱ, from which the Pareto fronts, the optimal technology combinations and operation conditions were obtained and analyzed. It's found that the system is feasible in both environmental and economic considerations after optimization. The most expensive processing section is decarbonization; the most expensive equipment is anaerobic digester; the most power-consuming processing section is digestion, followed by decarbonization and waste management. The positive green degree value on the process is attributed to processing section of digestion and waste management. 3:1 chicken feces and corn straw, solar energy, pressure swing adsorption and 3:1 chicken feces and rice straw, solar energy, pressure swing adsorption are turned out to be two robust technology combinations under different prices of methane and electricity by sensitivity analysis. The optimization results provide support for optimal design and operation of biogas production system considering environmental and economic objectives.

关键词： Biogas production system MINLP Multi-objective optimization Non-dominated sorting genetic algorithm Ⅱ green degree value

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Jahn–Teller Distortions Induced by in situ Li Migration in λ-MnO2for Boosting Electrocatalytic Nitrogen Fixation

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Angewandte Chemie 2023年第8期136卷

作者： Zijian Gao Zhi-hao Zhao Haifan Wang Yiling Bai Xuehua Zhang Zeyu Zhang Hui Mei Prof. Menglei Yuan Prof. Guangjin Zhang Chengdu Institute of Organic Chemistry Chinese Academy of Sciences Chengdu 610041 P. R. China Center of Materials Science and Optoeletronics Engineering Chinese Academy of Sciences Beijing 100049 P. R. China CAS Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P. R. China State Key Laboratory of Solidification Processing and School of Materials Science and Engineering Northwestern Polytechnical University Xi'an 710072 P. R. China State Key Laboratory of Coal Conversion CAS Key Laboratory of Carbon Materials Institute of Coal Chemistry Chinese Academy of Sciences Taiyuan 030001 P. R. China National Energy Center for Coal to Liquids Synfuels China Technology Co. Ltd Beijing 101400 P. R. China State Key Laboratory of Petroleum Molecular & Process Engineering(RIPP SINOPEC) Beijing 101407 P. R. China Queen Mary University of London Engineering School Northwestern Polytechnical University Xi'an 710129 P. R. China Key Laboratory of Green and High-value Utilization of Salt Lake Resources Chinese Academy of Sciences Beijing 100190 P. R. China

Lithium-mediated electrochemical nitrogen reduction reaction (Li-NRR) completely eschews the competitive hydrogen evolution reaction (HER) occurred in aqueous system, whereas the continuous deposition of lithium readily blocks the active sites and further reduces the reaction kinetics. Herein, we propose an innovative in situ Li migration strategy to realize that Li substitutes Mn sites in λ-MnO 2 instead of evolving into the dead Li. Comprehensive characterizations corroborate that the intercalation of Li + at high voltage breaks the structural integrity of MnO 6 octahedron and further triggers unique Jahn–Teller distortions, which promotes the spin state regulation of Mn sites to generate the ameliorative e g orbital configuration and accelerates N≡N bond cleavage via e g -σ and e g -π* interaction. To this end, the resulted cationic disordered LiMnO 4 delivers the recorded highest NH 3 yield rate of 220 μg h −1 cm −2 and a Faradaic efficiency (FE) 83.80 % in organic electrolyte.

关键词： Cationic Disordered LiMn2O4 Electrocatalytic Nitrogen Reduction Jahn–Teller Distortions Spin state Regulation in Situ Li Migration

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Direct low-temperature synthesis of ultralong persistent luminescence nanobelts based on a biphasic solution-chemical reaction

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Chinese Chemical Letters 2018年第11期29卷 1641-1644页

作者： Haoyang Liu Xiaoxia Hu Jie Wang Meng Liu Wei Wei Quan Yuan Key Laboratory of Analytical Chemistry for Biology and Medicine (Ministry of Education) College of Chemistry and Molecular SciencesWuhan University State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of Sciences

Here, we report the direct hydrothermal synthesis of 1 D-based Zn2GeO4：Mn2＋ persistent luminescent nanobelts （ZGO：Mn PLNBs）. The ZGO：Mn PLNBs exhibit rapid growth rate, and nanobelts can be obtained after 30 rain of hydrothermal treatment. The persistent luminescence performance can be fine-turned upon prolonging the hydrothermal time. Furthermore, the doping ratio of Mn2＋ exhibits influence on the persistent luminescence properties of ZGO：Mn PLNBs, and 2% doping of Mn2＋ shows superior persistent luminescence with decay time of longer than 20min. The developed 1D-based ZGO：Mn PLNBs can be simply prepared with the hydrothermal method and show tunable morphology and persistent luminescence. We believe that this solid-state-reaction-free chemical approach avoids the current key drawback in regard to PLNMs development, and thus will promote the broad use of these unique nanostructured PLNMs in developing optical device for imaging.

关键词： Hydrothermal Persistent luminescence Nanobelts Zinc germinate Mn ion

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Highly Selective CO2Electroreduction to Multi-Carbon Alcohols via Amine Modified Copper Nanoparticles at Acidic Conditions

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Angewandte Chemie 2024年第49期136卷

作者： Dr. Yahui Wu Prof. Dr. Chunjun Chen Prof. Dr. Shoujie Liu Prof. Dr. Qingli Qian Prof. Dr. Qinggong Zhu Dr. Rongjuan Feng Dr. Lihong Jing Prof. Dr. Xinchen Kang Prof. Dr. Xiaofu Sun Prof. Dr. Buxing Han Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Center for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences Beijing 100190 P. R. China School of Chemistry and Chemical Engineering University of Chinese Academy of Sciences Yuquan Road Shijingshan District Beijing 100049 P. R. China Shanghai Key Laboratory of Green Chemistry and Chemical Processes State Key Laboratory of Petroleum Molecular & Process Engineering School of Chemistry and Molecular Engineering East China Normal University Shanghai 200062 China School of Materials Science and Engineering Anhui University Hefei 230601 China

Electroreduction of CO 2 into multi-carbon (C2+) products (e.g. C2+ alcohols) offers a promising way for CO 2 utilization. Use of strong alkaline electrolytes is favorable to producing C2+ products. However, CO 2 can react with hydroxide to form carbonate/bicarbonate, which results in low carbon utilization efficiency and poor stability. Using acidic electrolyte is an efficient way to solve the problems, but it is a challenge to achieve high selectivity of C2+ products. Here we report that the amine modified copper nanoparticles exhibit high selectivity of C2+ products and carbon utilization at acidic condition. The Faradaic efficiency (FE) of C2+ products reach up to 81.8 % at acidic media (pH=2) with a total current density of 410 mA cm −2 over n-butylamine modified Cu. Especially the FE of C2+ alcohols is 52.6 %, which is higher than those reported for CO 2 electroreduction at acidic condition. In addition, the single-pass carbon efficiency towards C2+ production reach up to 60 %. Detailed studies demonstrate that the amine molecule on the surface of Cu cannot only enhance the formation, adsorption and coverage of *CO, but also provide a hydrophobic environment, which result in the high selectivity of C2+ alcohols at acidic condition.

关键词： carbon dioxide electrocatalysis multi-carbon alcohols acidic conditions green chemistry

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Lighting Up Bispyrene-Functionalized Chiral Molecular Muscles with Switchable Circularly Polarized Excimer Emissions

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Angewandte Chemie 2024年第1期137卷

作者： Xue Li Dr. Wei-Tao Xu Xiao-Qin Xu Dr. Yu Wang Dr. Xu-Qing Wang Prof. Dr. Hai-Bo Yang Prof. Dr. Wei Wang Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular Engineering East China Normal University 3663 N. Zhongshan Road Shanghai 200062 China State Key Laboratory of Petroleum Molecular and Process Engineering Sinopec Research Institute of Petroleum Processing Co. LTD. Beijing 100083 China East China Normal University Shanghai 200062 China Shanghai Center of Brain-inspired Intelligent Materials and Devices East China Normal University Shanghai 200241 China

Aiming at the further extension of the application scope of traditional molecular muscles, a novel bispyrene-functionalized chiral molecular [c2]daisy chain was designed and synthesized. Taking advantage of the unique dimeric interlocked structure of molecular [c2]daisy chain, the resultant chiral molecular muscle emits strong circularly polarized luminescence (CPL) attributed to the pyrene excimer with a high dissymmetry factor ( g lum ) value of 0.010. More importantly, along with the solvent- or anion- induced motions of the chiral molecular muscle, the precise regulation of the pyrene stacking within its skeleton results in the switching towards either “inversed” state with sign inversion and larger g lum values or “down ” state with maintained handedness and smaller g lum values, making it a novel multistate CPL switch. As the first example of chiral molecular muscle-based CPL switch, this proof-of-concept study not only successfully widens the application scopes of molecular muscles, but also provides a promising platform for the construction of novel smart chiral luminescent materials for practical applications.

关键词： molecular machine molecular daisy chain pillar[5]arene pyrene excimer stimuli responsiveness

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Intermittent electrolysis enabling the enhanced efficiency and stability for nitrate reduction

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Chem 2025年

作者： Limin Wu Libing Zhang Jiaqi Feng Shunhan Jia Ruhan Wang Xinning Song Xiaodong Ma Qinggong Zhu Xinchen Kang Qingli Qian Xiaofu Sun Buxing Han Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Center for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China School of Chemical Sciences University of Chinese Academy of Sciences Beijing 100049 China College of Chemical Engineering and Environment China University of Petroleum Beijing 102249 China Shanghai Key Laboratory of Green Chemistry and Chemical Processes State Key Laboratory of Petroleum Molecular & Process Engineering School of Chemistry and Molecular Engineering East China Normal University Shanghai 200062 China Institute of Eco-Chongming 20 Cuiniao Road Chenjia Town Chongming District Shanghai 202162 China

Catalyst deactivation is a common issue in catalysis, which restricts its practical applications. Nitrate electroreduction using copper (Cu) catalysts offers an eco-friendly NH 3 production route. However, the NH 3 selectivity and activity decline significantly due to Cu surface reconstruction and compositional changes during electrolysis. Herein, an intermittent reduction strategy is proposed to maintain high efficiency and stability of Cu 2 O for NO 3 − to NH 3 through applying an alternating on/off electrolysis. The high Faradaic efficiency (FE) (≥90%) and current density (≥110 mA cm −2 ) were maintained at least 200 h, which improved the cycle stability by 40 times compared with relay electrolysis. Detailed experimental studies and theoretical calculations manifest that the composition and structure of Cu catalyst could be recovered periodically via intermittent electrolysis, which facilitated NO 3 − adsorption, moderated ∗NO 2 coverage, and balanced ∗H production/consumption, leading to high selectivity toward NH 3 in long-term electrolysis. Further investigation showed that this strategy could also be extended to other Cu-based catalysts.

关键词： ammonia synthesis electrocatalysis green chemistry nitrate reduction SDG11: Sustainable cities and communities SDG6: Clean water and sanitation

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Highly Efficient Electrocatalytic CO2Reduction to C2+Products on a Poly(ionic liquid)-Based Cu0–CuITandem Catalyst

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Angewandte Chemie 2021年第9期134卷

作者： Dr. Guo-Yi Duan Xiao-Qiang Li Guang-Rong Ding Prof. Dr. Li-Jun Han Prof. Dr. Bao-Hua Xu Prof. Dr. Suo-Jiang Zhang Beijing Key Laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China School of Chemical Engineering University of Chinese Academy of Sciences Beijing 100049 China

Electroreduction of CO 2 on a polymer-modified Cu-based catalyst has shown high multi-electron reduction (>2 e − ) selectivity, however, most of the corresponding current densities are still too small to support industrial applications. In this work, we designed a poly(ionic liquid) (PIL)-based Cu 0 –Cu I tandem catalyst for the production of C 2+ products with both high reaction rate and high selectivity. Remarkably, a high C 2+ faradaic efficiency (FE ) of 76.1 % with a high partial current density of 304.2 mA cm −2 is obtained. Mechanistic studies reveal the numbers and highly dispersed Cu 0 -PIL-Cu I interfaces are vital for such reactivity. Specifically, Cu nanoparticles derived Cu 0 -PIL interfaces account for high current density and a moderate C 2+ selectivity, whereas Cu I species derived PIL-Cu I interfaces exhibit high activity for C−C coupling with the local enriched *CO intermediate. Furthermore, the presence of the PIL layer promotes the C 2+ selectivity by lowering the barrier of C−C coupling.

关键词： CO2 conversion Electrochemistry Ionic liquids Polymer modification Tandem catalyst

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Energy consumption simulation and diagnosis in the coking process: A mechanism and data-driven approach

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Energy for Sustainable Development 2025年 88卷

作者： Yangmei Ji Gang Sheng Qi Zhang Jialin Shen State Environmental Protection Key Laboratory of Eco-Industry Northeastern University Shenyang 110819 China State Key Laboratory of Metallurgical Intelligent Manufacturing System Automation Research and Design Institute of Metallurgical Industry Co. Ltd. Beijing 100071 China Central Iron & Steel Research Institute Beijing 100071 China Engineering Research Center of Ministry of Education for Frontier Technologies of Low-Carbon Steelmaking Shenyang 110819 Liaoning China Liaoning Province Engineering Research Center for Energy Saving and Green Low Carbon Technologies in Process Industry Shenyang 110819 Liaoning China

With the enhancement of energy resources and environmental constraints, key energy-consuming industries, such as the steel industry, must urgently achieve an efficient transformation of energy conservation. The energy consumption is influenced by multiple factors, including operating parameters, energy utilization methods, and energy-saving technologies in steel enterprises, with its variation levels exhibiting complexity and regularity. However, the underlying mechanisms driving energy consumption fluctuations remain unclear, and there is a lack of real-time collaborative control strategies adapted to actual production scenarios. Moreover, the energy-saving potential of existing technologies and the energy-saving effects after technological retrofit remain uncertain. To address these challenges, this study develops an energy consumption simulation and diagnostic model based on both mechanism and data-driven approaches. The model simulates the fluctuation trends of energy consumption and identifies key influencing factors, thereby providing targeted operational optimization suggestions. Taking the coking process as a case study, a hierarchical diagnostic approach is applied to evaluate the energy consumption level by selecting the minimum energy consumption value for 30 days as the benchmark. The analysis identifies that the coal composition is the most effective controllable factor. Adjusting key coal parameters is expected to reduce energy consumption by 3.60 kgce/t. Furthermore, deploying new energy-saving technologies can further decrease energy consumption by 4.27 kgce/t. In summary, this research provides a technical framework and practical guidance for the benchmarking of energy efficiency of steel enterprises.

关键词： Mechanism and data-driven Energy diagnosis Energy consumption simulation Optimization suggestions Technical potential assessment Coking process

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Switching CO2Electroreduction Pathways between Ethylene and Ethanol via Tuning Microenvironment of the Coating on Copper Nanofibers

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Angewandte Chemie 2024年第1期137卷

作者： Xing Tong Pei Zhang Peng Chen Zhuosen He Xinchen Kang Yaoyu Yin Yingying Cheng Meng Zhou Lihong Jing Ce Wang Baocai Xu Lirong Zheng Xueqing Xing Zhonghua Wu Buxing Han Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Center for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Science Beijing 100190 China School of Chemistry University of Chinese Academy of Sciences Beijing 100049 China Beijing Technology and Business University School of Light Industry Science and Engineering Beijing 100048 China Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China Shanghai Key Laboratory of Green Chemistry and Chemical Processes State Key Laboratory of Petroleum Molecular & Process Engineering School of Chemistry and Molecular Engineering East China Normal University Shanghai 200062 China

engineering the microenvironment of electrode surface is one of the effective means to tune the reaction pathways in CO 2 RR. In this work, we prepared copper nanofibers with conductive polypyrrole coating by polymerization of pyrrole using polyvinyl pyrrolidone (PVP) as template. As a result, the obtained copper nanofibers Cu/Cu 2+1 O/SHNC, exhibited a superhydrophobic surface, which demonstrated very high selectivity for ethanol with a Faraday efficiency (FE) of 66.5 % at −1.1 V vs reversible hydrogen electrode (RHE) in flow cell. However, the catalyst Cu/Cu 2+1 O/NC, which was prepared under the same conditions but without PVP, possessed a hydrophobic surface and exhibited high selectivity towards ethylene at the given potentials. The mechanism for switch of reaction pathways from ethylene to ethanol in CO 2 RR was studied. Incorporating pyrrolidone groups into the polymer coating results in the formation of a superhydrophobic surface. This surface weakens the hydrogen bonding interaction between interfacial water molecules and facilitates the transfer of CO 2 , thereby enhancing the local CO 2 /H 2 O ratio. The high coverage of *CO promotes the coupling of *CO and *CHO to form C 2 intermediates, and reduces the reaction energy for the formation of *CHCHOH (ethanol path) at the interface. This ensures that the reaction pathway is directed towards ethanol.

关键词： CO2 electroreduction reaction pathways ethanol interfacial microstructure superhydrophobic surface

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Sodium Dithionite-Mediated Decarboxylative Sulfonylation: Facile Access to Tertiary Sulfones

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Advanced Materials 2020年第23期59卷 8992-8996页

作者： Li, Yaping Chen, Shihao Wang, Ming Jiang, Xuefeng Shanghai Key Laboratory of Green Chemistry and Chemical Process School of Chemistry and Molecular Engineering East China Normal University 3663 North Zhongshan Road Shanghai200062 China State Key Laboratory of Elemento-organic Chemistry Nankai University Tianjin300071 China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic Chemistry Chinese Academy of Sciences 345 Lingling Road Shanghai200032 China

A straightforward multicomponent decarboxylative cross coupling of redox-active esters (N-hydroxyphthalimide ester), sodium dithionite, and electrophiles was established to construct sterically bulky sulfones. The inorganic salt sodium dithionite not only served as the sulfur dioxide source, but also acted as an efficient radical initiator for the decarboxylation. Notably, diverse naturally abundant carboxylic acids and artificially prepared carboxyl-containing drugs with multiple heteroatoms and sensitive functional groups successfully underwent this decarboxylative sulfonylation to provide sterically bulky tertiary sulfones. Mechanistic studies further demonstrated that decarboxylation was the rate-determining step and occurred via a single-electron transfer (SET) process with the assistance of sodium dithionite. © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

关键词： Esters

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