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CO_(2)capture costs of chemical looping combustion of biomass:A comparison of natural and synthetic oxygen carrier

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Journal of Energy Chemistry 2024年第5期92卷 296-310页

作者： Benjamin Fleiß Juraj Priscak Martin Hammerschmid Josef Fuchs Stefan Müller Hermann Hofbauer Institute of Chemical Environmental and Bioscience EngineeringTU WienVienna1060 ViennaAustria BEST–bioenergy and Sustainable Technologies GmbH Graz8010 StyriaAustria

Chemical looping combustion has the potential to be an efficient and low-cost technology capable of contributing to the reduction of the atmospheric concentration of CO_(2) in order to reach the 1.5/2°C goal and mitigate climate *** this process,a metal oxide is used as oxygen carrier in a dual fluidized bed to generate clean CO_(2) via combustion of *** commonly,natural ores or synthetic materials are used as oxygen carrier whereas both must meet special requirements for the conversion of solid *** oxygen carriers are characterized by higher reactivity at the expense of higher costs versus the lower-cost natural *** determine the viability of both possibilities,a techno-economic comparison of a synthetic material based on manganese,iron,and copper to the natural ore ilmenite was *** synthetic oxygen carrier was characterized and tested in a pilot plant,where high combustion efficiencies up to 98.4%and carbon capture rates up to 98.5%were *** techno-economic assessment resulted in CO_(2) capture costs of 75 and 40€/tCO_(2) for the synthetic and natural ore route respectively,whereas a sensitivity analysis showed the high impact of production costs and attrition rates of the synthetic *** synthetic oxygen carrier could break even with the natural ore in case of lower production costs and attrition rates,which could be reached by adapting the production process and recycling *** comparison to state-of-the-art technologies,it is demonstrated that both routes are viable and the capture cost of CO_(2) could be reduced by implementing the chemical looping combustion technology.

关键词： Chemical looping combustion BECCS Techno-economic assessment CO_(2)capture costs Oxygen carrier development Synthetic materials Ilmenite

Efficient ammonia production over e_(g)-occupancy-optimized perovskite electrocatalysts

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Nano Research 2024年第6期17卷 4682-4686页

作者： Mingfa Chen Yu Zhang Fulong Liu Zhenbao Zhang Yuming Dong Yongfa Zhu Heqing Jiang Jiawei Zhu Key Laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi 214122China Qingdao Institute of bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266101China School of Chemistry and Chemical engineering Linyi UniversityLinyi 276005China department of Chemistry Tsinghua UniversityBeijing 100084China

Renewable-energy-driven nitrate(NO_(3)^(−))electroreduction to ammonia(NH_(3))(NERA)has been an attractive technology for decarbonizing NH_(3)production and wastewater *** NERA efficiency requires electrocatalysts that are earth-abundant and show fantastic *** we report a semiempirical activity descriptor of eg occupancy(of surface B-site cations)for identifying inexpensive perovskite oxides with extremely high efficacy toward *** establish the descriptor by systematic investigations of more than 10 perovskite *** investigations demonstrate that their intrinsic NERA activities display a volcano-shaped dependence on eg occupancy and the optimized intrinsic activities are accessible at near-1 eg *** could plausibly be attributed to the favorable overlaps between surface adsorbates and vertically-oriented eg *** importantly,utilizing this descriptor,we predict a highly active,selective,and durable NERA electrocatalyst with a composition of Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3−δ)(BSCF).Because of its close-to-1 e_(g)occupancy(i.e.~1.2),the BSCF features a superior NH_(3)production rate of 0.12 g·h^(−1)·mg_(cat.)^(−1)(Faradaic efficiency of 97.8%)that is at top of the volcano plot,and substantially outperforms most NERA electrocatalysts reported in literature.

关键词： perovskite oxide nitrate electroreduction ammonia electrosynthesis eg occupancy

Hydrogen spillover bridged dual nano-islands triggered by built-in electric field for efficient and robust alkaline hydrogen evolution at ampere-level current density

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Nano Research 2024年第6期17卷 5050-5060页

作者： Kecheng Tong Liangliang Xu Hanxu Yao Xingkun Wang Canhui Zhang Fan Yang Lei Chu Jinwoo Lee Heqing Jiang Minghua Huang School of Materials Science and engineering Ocean University of ChinaQingdao 266100China department of Chemical and Biomolecular engineering Korea Advanced Institute of Science and Technology(KAIST)291Daejeon 34141Republic of Korea Qingdao New Energy Shandong Laboratory Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101China University of Chinese Academy of Sciences Beijing 100049China

Employing the alkaline water electrolysis system to generate hydrogen holds great prospects but still poses significant challenges,particularly for the construction of hydrogen evolution reaction(HER)catalysts operating at ampere-level current ***,the unique Ru and RuP_(2)dual nano-islands are deliberately implanted on N-doped carbon substrate(denoted as Ru-RuP_(2)/NC),in which a built-in electric field(BEF)is spontaneously generated between Ru-RuP_(2)dual nano-islands driven by their work function *** and theoretical results unveil that such constructed BEF could serve as the driving force for triggering fast hydrogen spillover process on bridged Ru-RuP_(2)dual nano-islands,which could invalidate the inhibitory effect of high hydrogen coverage at ampere-level current density,and synchronously speed up the water dissociation on Ru nano-islands and hydrogen adsorption/desorption on RuP_(2)nano-islands through hydrogen spillover *** a result,the Ru-RuP_(2)/NC affords an ultra-low overpotential of 218 mV to achieve 1.0 A·cm^(−2)along with the superior stability over 1000 h,holding the great promising prospect in practical applications at ampere-level current *** importantly,this work is the first to advance the scientific understanding of the relationship between the constructed BEF and hydrogen spillover process,which could be enlightening for the rational design of the cost-effective alkaline HER catalysts at ampere-level current density.

关键词： built-in electric field hydrogen spillover dual nano-islands ampere-level current density alkaline hydrogen evolution

Carbene chemistry for unnatural biosynthesis

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Science China(Life Sciences) 2024年第1期67卷 204-207页

作者： Jing Huang Jay D.Keasling department of Chemical and Biomolecular engineering University of CaliforniaBerkeley 94720USA Joint bioenergy Institute Lawrence Berkeley National LaboratoryEmeryville 94608USA Biological Systems and engineering Division Lawrence Berkeley National LaboratoryBerkeley 94720USA Novo Nordisk Foundation Center for Biosustainability Technical University of DenmarkKongens Lyngby 2800Denmark department of Bioengineering University of CaliforniaBerkeley 94720USA Synthetic Biochemistry Center Institute for Synthetic BiologyShenzhen Institutes for Advanced TechnologiesShenzhen 518055China

Previously,chemists working in synthesis were jealous of biologists since the enzymes found in nature usually exhibited great catalytic properties(e.g.,high catalytic efficiency,excellent selectivity such as substrate selectivity,regioselectivity and stereoselectivity).However,biological systems lack many counterparts of reactions widely used in chemical synthesis.

关键词： synthesis selectivity catalytic

Strong metal–support interaction boosts the electrocatalytic hydrogen evolution capability of Ru nanoparticles supported on titanium nitride

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Carbon Energy 2024年第1期6卷 245-254页

作者： Xin Wang Xiaoli Yang Guangxian Pei Jifa Yang Junzhe Liu Fengwang Zhao Fayi Jin Wei Jiang Haoxi Ben Lixue Zhang College of Chemistry and Chemical engineering Collaborative Innovation Center for Hydrogen Energy Key Materials and Technologies of Shandong ProvinceQingdao UniversityQingdaoShandongChina State Key Laboratory of Bio-fibers and Eco-Textiles Qingdao UniversityQingdaoShandongChina Qingdao Institute of bioenergy and Bioprocess Technology Chinese Academy of ScienceQingdaoShandongChina

Ruthenium(Ru)has been regarded as one of the most promising alternatives to substitute Pt for catalyzing alkaline hydrogen evolution reaction(HER),owing to its inherent high activity and being the cheapest platinum-group ***,based on the idea of strong metal–support interaction(SMSI)regulation,Ru/TiN catalysts with different degrees of TiN overlayer over Ru nanoparticles were fabricated,which were applied to the alkaline electrolytic *** reveal that the TiN overlayer would gradually encapsulate the Ru nanoparticles and induce more electron transfer from Ru nanoparticles to TiN support by the Ru–N–Ti bond as the SMSI degree *** study shows that the exposed Ru–TiN interfaces greatly promote the H_(2) desorption ***,the Ru/TiN-300 with a moderate SMSI degree exhibits excellent HER performance,with an overpotential of 38 mV at 10 mA cm^(−2).Also,due to the encapsulation role of TiN overlayer on Ru nanoparticles,it displays super long-term stability with a very slight potential change after 24 *** study provides a deep insight into the influence of the SMSI effect between Ru and TiN on HER and offers a novel approach for preparing efficient and stable HER electrocatalysts through SMSI engineering.

关键词： electronic structure hydrogen evolution reaction ruthenium strong metal-support interaction titanium nitride

Ethanol steam reforming over Ni/ZSM-5 nanosheet for hydrogen production

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Chinese Journal of Chemical engineering 2024年第3期67卷 247-256页

作者： Porapak Suriya Shanshan Xu Shengzhe Ding Sarayute Chansai Yilai Jiao Joseph Hurd Daniel Lee Yuxin Zhang Christopher Hardacre Prasert Reubroycharoen Xiaolei Fan department of Chemical engineering School of EngineeringThe University of ManchesterManchester M139PLUnited Kingdom Program of Petrochemistry and Polymer Science Faculty of ScienceChulalongkorn UniversityBangkok10330Thailand Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China Liaoning Academy of Materials Shenyang 110167China Center of Excellence in Catalysis for bioenergy and Renewable Chemicals(CBRC) andDepartment of Chemical TechnologyFaculty of ScienceChulalongkorn UniversityBangkok 10330Thailand Nottingham Ningbo China Beacons of Excellence Research and Innovation Institute University of Nottingham Ningbo ChinaNingbo315100China

Compared to reforming reactions using hydrocarbons,ethanol steam reforming(ESR)is a sustainable alternative for hydrogen(H_(2))production since ethanol can be produced sustainably using *** work explores the catalyst design strategies for preparing the Ni supported on ZSM-5 zeolite catalysts to promote ***,two-dimensional ZSM-5 nanosheet and conventional ZSM-5 crystal were used as the catalyst carriers and two synthesis strategies,i.e.,in situ encapsulation and wet impregnation method,were employed to prepare the *** on the comparative characterization of the catalysts and comparative catalytic assessments,it was found that the combination of the in situ encapsulation synthesis and the ZSM-5 nanosheet carrier was the effective strategy to develop catalysts for promoting H_(2) production via ESR due to the improved mass transfer(through the 2-D structure of ZSM-5 nanosheet)and formation of confined small Ni nanoparticles(resulted via the in situ encapsulation synthesis).In addition,the resulting ZSM-5 nanosheet supported Ni catalyst also showed high Ni dispersion and high accessibility to Ni sites by the reactants,being able to improve the activity and stability of catalysts and suppress metal sintering and coking during ESR at high reaction ***,the Ni supported on ZSM-5 nanosheet catalyst prepared by encapsulation showed the stable performance with~88% ethanol conversion and~65% H_(2) yield achieved during a 48-h longevity test at 550-C.

关键词： ZSM-5 nanosheet In situ encapsulation Ni catalyst Ethanol steam reforming Hydrogen production

Bonding Interaction of Adjacent Pt and Ag Single-Atom Pairs on Carbon Nitride Efficiently Promotes Photocatalytic H_(2)Production

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CCS Chemistry 2024年第6期6卷 1523-1534页

作者： Guanchao Wang Chaofan Zhang Wantong Zhao Baojun Wang Yuefeng Liu Ting Zhang Wenguang Cui Riguang Zhang Zhongkui Zhao State Key Laboratory of Fine Chemicals Department of Catalysis Chemistry and EngineeringSchool of Chemical EngineeringDalian University of TechnologyDalian 116024 State Key Laboratory of Clean and Efficient Coal Utilization College of Chemical Engineering and TechnologyTaiyuan University of TechnologyTaiyuan 030024 Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023 CAS Key Laboratory of Bio-Based Materials Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101 College of Chemical engineering Shijiazhuang UniversityShijiazhuang 050035

Dual-atom catalysts(DACs)represent an exciting advance in the field of heterogeneous *** not only retain the beneficial characteristics of single-atom catalysts(SACs),but they also harness the synergistic effects that arise from the proximity of neighboring single-metal ***,the fabrication of heteronuclear dual-atom metals positioned adjacently for use in photocatalysis remains a significant ***,we report the atomically dispersed adjacent Pt-Ag dual-atom pairs on carbon nitride(Pt1Ag1-a/CN)by a facile hydrogen-bonding assembly strategy via pyrolysis of the hydrogen-bonding supramolecule containing melamine-Ag and cyanuric acid-Pt complexes on carbon nitride(CN),through which the light absorption depressed by deposited carbonaceous materials during the preparation of dual-atom metals via a traditional method like the pyrolysis of the metal-organic *** to the synergism achieved by the bonding interaction of adjacent Pt and Ag single-atom pairs,the developed Pt1Ag1-a/CN with 0.21%Pt loading shows a high turnover frequency(TOF)of 1115 h^(−1)with a H_(2)evolution rate(HER)of 12,000μmol g^(−1)h^(−1)for photocatalytic water splitting under simulated solar light irradiation(325 h^(−1)of TOF with 3480μmol g^(−1)h^(−1)of HER under visible light irradiation).This strategy outperforms the previously reported SACs on CN-based *** functional theory(DFT)calculations demonstrate that the adjacent Ag atom acts as a coordination atom to effectively regulate the electronic structure of the Pt atom and thus brings the d-band center of Pt close to the Fermi energy level,which is beneficial for the H_(2)*** work presents a facile and general strategy for designing diverse adjacent diatomic cocatalysts in photocatalysis without depressing light absorption by the deposited carbon during the DAC preparation via previously reported methods.

关键词： dual-atom metal catalysts synergistic effect graphitic carbon nitride hydrogen evolution photocatalysis

Simultaneously optimizing exciton diffusion length and nonradiative energy loss in organic solar cells via ternary strategy

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Science China Chemistry 2024年第9期67卷 3004-3011页

作者： Huanxiang Jiang Hao Lu Zezhou Liang Yonghai Li Guangliu Ran Chenyu Han Yuqiang Liu Hongxiang Li Xichang Bao Zhishan Bo College of Textiles and Clothing State Key Laboratory of Bio-fibers and Eco-textilesQingdao UniversityQingdao 266071China Qingdao Institute of bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266101China Key Laboratory for Physical Electronics and Devices of the Ministry of Education&Shaanxi Key Lab of Photonic Technique for InformationSchool of Electronics Science&EngineeringFaculty of Electronic and Information EngineeringXi’an Jiaotong UniversityXi’an 710049China department of Physics and Applied Optics Beijing Area Major Laboratory Center for Advanced Quantum StudiesBeijing Normal UniversityBeijing 100875China College of Polymer Science and engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065China Laboratory of Solar Energy Shandong Energy InstituteQingdao 266101China

Significant nonradiative energy loss and short exciton diffusion length in organic solar cells(OSCs)are two major obstacles to achieving state-of-the-art *** is crucial to conduct a study on the intensive mechanism and improvement strategies for future breakthroughs in the efficiency of *** this work,nonradiative energy loss and exciton diffusion length are optimized simultaneously by incorporating a guest acceptor(LA15)to construct ternary OSC(D18:L8-BO:LA15).Firstly,LA15 exhibits excellent compatibility with the host acceptor L8-BO,and effectively improves the fluorescence quantum efficiency(FLQY),resulting in suppressed non-radiative energy ***,LA15 effectively prolongs the fluorescent lifetime of the acceptor phase from 0.85 to 1.12 ns,leading to larger exciton diffusion length,which is beneficial for reducing geminate ***,the addition of LA15 optimizes the crystallinity of the active layer with amplified charge transport *** a result,the optimized D18:L8-BO:LA15 device achieves ultralow nonradiative energy loss of 0.18 e V and improved fill factor(FF)with high efficiency up to 19.13%.These results highlight the crucial roles of regulating FLQYand exciton lifetime in achieving highefficiency OSCs.

关键词： organic solar cells nonradiative energy loss exciton lifetime exciton diffusion length

Degradation pathways of amino acids during thermal utilization of biomass: a review

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Frontiers of Chemical Science and engineering 2024年第7期18卷 67-95页

作者： Mubarak Al-Kwradi Mohammednoor Altarawneh department of Chemical and Petroleum engineering United Arab Emirates UniversityAl-Ain 15551United Arab Emirates

Amino acids are important nitrogen carriers in biomass and entail a broad spectrum of industrial uses,most notably as food additives,pharmaceutical ingredients,and raw materials for bio-based *** detailed information in regard to the fragmentation of amino acids is essential to comprehend the nitrogen transformation chemistry at conditions encountered during hydrothermal and pyrolytic degradation of *** underlying aim of this review is to survey literature studies pertinent to the complex structures of amino acids,their formation yields from various categories of biomass,and their fragmentation routes at elevated temperatures and in the aqueous *** predominant degradation reactions ensue in the decomposition of amino acids,namely deamination and ***,minor differences in structure can greatly affect the fate for each amino ***,amino acids,being nitrogen-rich compounds,play pivotal roles across various *** is a growing interest in producing varied types and configurations of amino *** fermentation appears to a viable approach to produce amino acids at an industrial *** innovative method under investigation is catalytic synthesis using renewable biomass as *** a method taps into the inherent nitrogen in biomass sources like chitin and proteins,eliminating the need for external nitrogen *** environmentally friendly approach is in line with green chemistry principles and has been gathering momentum in the scientific community.

关键词： amino acids pyrolysis biomass nitrogen mechanisms bioenergy