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

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

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Laser-assisted grinding of RB-SiC composites:Laser ablation behavior and mechanism

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Chinese journal of Aeronautics 2024年第1期37卷 362-376页

作者： Zhigang dong Wenchao SUN Xintong CAI Feng YANG Yan BAO Renke KANG dongjiang WU Guangyi MA Fangyong NIU Key Laboratory for Precision and Non-traditional Machining Technology of the Ministry of Education School of Mechanical EngineeringDalian University of TechnologyDalian 116024China

Laser ablation is an important process during Laser-Assisted Grinding(LAG)of hard and brittle *** realize controllable material removal during laser ablation of RB-SiC composites,ablation experiments under different Laser Energy Density(LAED)and LAG experiments are *** rules and mechanism of physical phase,ablation morphology and crack characteristics caused by laser irradiation are *** forces of LAG and Conventional Grinding(CG)are *** results show that ablation surface changes from slight oxidation to obvious material removal with LAED increasing,and ablation depth increases *** ablation products change from submicron SiO_(2)particles to nanoscale particles and *** LAED promotes SiC decomposition and sublimation,which leads to the increase of C *** SiC phase forms corrugated shape in recast layer and columnar shape in heat Affected Zone(hAZ)at 56 j/mm^(2).The cold and heat cycle leads to formation of fishbone *** ablation specimen under 30 j/mm^(2),the grinding force can be reduced by a maximum of 39%and brittle damage region is *** material removal and microcrack generated will significantly reduce the hardness and improve machinability,which can promote grinding efficiency.

关键词： RB-SiC Laser Ceramic Composites Grinding

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Improvement of impact properties of Al-Si-Mg alloy via solution treatment and joint modification with Sr and La

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Rare Metals 2024年第7期43卷 3301-3313页

作者： Xiong-Ling Zheng Shao-Xiang Li jia-Le Ma Qing-Yan Xu hai-dong Zhao Zhi-Qiang han Key Laboratory for Advanced Materials Processing Technology Ministry of EducationSchool of Materials Science and EngineeringTsinghua UniversityBeijing 100084China National Engineering Research Center of Near-Net Shape Forming for Metallic Materials South China University of TechnologyGuangzhou 510641China

An effort to obtain superior impact properties for Al-7Si-0.35 Mg alloy is presented,where modification with 0.02 wt% Sr and 0.1 wt% La as well as solution treatment was jointly *** samples were solution treated at 535℃ for 15 min to 12 *** microstructure,fracture mechanism,and their correlation with the impact properties of the alloy were studied in detail mainly through optical microscopy(OM),scanning electron microscopy(SEM) and oscillography impact *** results show that the addition of Sr and La refined the eutectic Si particles significantly from~ 2.05 μm(modified with Sr alone) to~ 0.75 μm in as-cast microstructure,leading to a very homogeneous distribution of spheroidized Si particles in the alloy solution treated at 535℃ for 8 *** alloy exhibits excellent impact toughness up to 75 j·cm^(-2),which is much higher than the maximum impact toughness of the alloys modified by Sr alone(~ 46 j·cm^(-2)).The major reason for this remarkable increase in the impact property is the dramatic increase in crack initiation *** dispersoid-free zones(DFZs)near the eutectic regions mainly consist of the ductile Al-matrix,which exhibits excellent *** ductile Al-matrix of the DFZs hinders the crack propagation,resulting in a significant increase in crack propagation energy.

关键词： Aluminum alloys Modification Solution treatment Microstructure Impact properties Fracture mechanism

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Nano-Ni-Induced Electronic Modulation of MoS_(2) Nanosheets Enables Energy-Saving h_(2) Production and Sulfide Degradation

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Energy & Environmental Materials 2024年第3期7卷 228-235页

作者： Fan Liu Xinghong Cai Yang Tang Wenqian Liu Qianwei Chen Peixin dong Maowen Xu Yangyang Tan Sh.j.an Bao Institute for Clean Energy&Advanced Materials School of Materials and EnergySouthwest UniversityChongqing 400715China

Electrocatalytic hydrogen evolution and sulfion(S^(2-))recycling are promising strategies for boosting h_(2)production and removing environmental ***,a nano-Ni-functionalized molybdenum disulfide(MoS_(2))nanosheet was assembled on steel mesh(Ni-MoS_(2)/SM)for use in sulfide oxidation reaction-assisted,energy-saving h_(2)*** and theoretical calculation results revealed that anchoring nano-Ni on high-surface-area slack MoS_(2)nanosheets not only optimized catalyst adsorption of polysulfides but also played an important role in promoting hydrogen evolution reaction kinetics by absorbing Oh_(ad),thereby greatly enhancing the catalytic performance toward sulfide oxidation reaction and hydrogen evolution ***,the Ni/MoS^(2-)based hydrogen evolution reaction+sulfide oxidation reaction system achieved nearly 100%hydrogen production efficiency and only consumed 61%less power per kWh than the oxygen evolution reaction+hydrogen evolution reaction system,which suggested our proposed Ni-MoS_(2)and novel hydrogen production system are promising for sustainable energy production.

关键词： hydrogen evolution reaction low energy consumption molybdenum disulfide sulfide oxidation reaction

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Deep Insight of Design,Mechanism,and Cancer Theranostic Strategy of Nanozymes

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Nano-Micro Letters 2024年第2期16卷 165-217页

作者： Lu Yang Shuming dong Shili Gai Dan Yang he Ding Lili Feng Guixin Yang Ziaur Rehman Piaoping Yang Key Laboratory of Superlight Materials and Surface Technology Ministry of EducationCollege of Materials Science and Chemical EngineeringHarbin Engineering UniversityHarbin 150001People’s Republic of China Yantai Research Institute Harbin Engineering UniversityYantai 264000People’s Republic of China Key Laboratory of Green Chemical Engineering and Technology of heilongjiang Province College of Material Science and Chemical EngineeringHarbin University of Science and TechnologyHarbin 150040People’s Republic of China Department of Chemistry Quaid-i-Azam UniversityIslamabad 45320Pakistan

Since the discovery of enzyme-like activity of Fe3O4 nanoparticles in 2007,nanozymes are becoming the promising substitutes for natural enzymes due to their advantages of high catalytic activity,low cost,mild reaction conditions,good stability,and suitable for large-scale ***,with the cross fusion of nanomedicine and nanocatalysis,nanozyme-based theranostic strategies attract great attention,since the enzymatic reactions can be triggered in the tumor microenvironment to achieve good curative effect with substrate specificity and low side ***,various nanozymes have been developed and used for tumor *** this review,more than 270 research articles are discussed systematically to present progress in the past five ***,the discovery and development of nanozymes are ***,classification and catalytic mechanism of nanozymes are ***,activity prediction and rational design of nanozymes are focused by highlighting the methods of density functional theory,machine learning,biomimetic and chemical ***,synergistic theranostic strategy of nanozymes are ***,current challenges and future prospects of nanozymes used for tumor theranostic are outlined,including selectivity,biosafety,repeatability and stability,in-depth catalytic mechanism,predicting and evaluating activities.

关键词： Nanozymes Classification Prediction and design Catalytic mechanism Tumor theranostics

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Multifunctional MOF@COF Nanoparticles Mediated Perovskite Films Management Toward Sustainable Perovskite Solar Cells

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Nano-Micro Letters 2024年第9期16卷 195-208页

作者： Yayu dong jian Zhang hongyu Zhang Wei Wang Boyuan hu Debin Xia Kaifeng Lin Lin Geng Yulin Yang MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangPeople’s Republic of China School of Materials Science and Engineering East China Jiaotong UniversityNanchang 330013JiangxiPeople’s Republic of China School of Materials Science and Engineering Harbin Institute of TechnologyHarbin 150001HeilongjiangPeople’s Republic of China

Although covalent organic frameworks(COFs)with highπ-conjugation have recently exhibited great prospects in perovskite solar cells(PSCs),their further application in PSCs is still hindered by face-to-face stacking and aggregation ***,metal-organic framework(MOF-808)is selected as an ideal platform for the in situ homogeneous growth of a COF to construct a core-shell MOF@COF nanoparticle,which could effectively inhibit COF stacking and *** synergistic intrinsic mechanisms induced by the MOF@COF nanoparticles for reinforcing intrinsic stability and mitigating lead leakage in PSCs have been *** complementary utilization ofπ-conjugated skeletons and nanopores could optimize the crystallization of large-grained perovskite films and eliminate *** resulting PSCs achieve an impressive power conversion efficiency of 23.61%with superior open circuit voltage(1.20 V)and maintained approximately 90%of the original power conversion efficiency after 2000 h(30-50%Rh and 25-30℃).Benefiting from the synergistic effects of the in situ chemical fixation and adsorption abilities of the MOF@COF nanoparticles,the amount of lead leakage from unpackaged PSCs soaked in water(he laboratory assessment required for the Resource Conservation and Recovery Act Regulation.

关键词： Perovskite solar cells Covalent organic frameworks Metal-organic frameworks Lead leakage Stability

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Amine-functionalized metal organic framework@graphene oxide as filler in PAEK-containing carboxyl group membrane for ultrafiltration with ultra-high permeability and strong fouling resistance

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Chinese journal of Chemical Engineering 2024年第6期70卷 93-103页

作者： Zhaoli Wang Wenjing Li Yi Zhang Yanyin Cheng junjian Yu Tianming dong Xiaoyu Chi Di Liu Zhe Wang School of Chemistry and Life Science Changchun University of TechnologyChangchun 130012China Advanced Institute of Materials Science Changchun University of TechnologyChangchun 130012China Key Laboratory of Advanced Functional Polymer Membrane Materials of jilin Province Changchun 130012China

Achieving high fouling resistance and permeability using membrane separation technology in water treatment processes remains a *** this work,a novel mixed-matrix membrane(MMM)(poly(arylene ether ketone)[PAEK]-containing carboxyl groups[PAEK-COOh]/UiO-66-Nh_(2)@graphene oxide[GO])with superb fouling resistance and high permeability was prepared by the nonsolvent-induced phase separation method,by in-situ growth of UiO-66-Nh_(2) on the GO layer,and by preparing hydrophilic *** the basis of the structure and performance analysis of the MMM,the maximum water flux reached 591.25 L·m^(-2)·h^(-1) for PAEK-COOh/UiO-66-Nh_(2)@GO,whereas the retention rate for bovine serum albumin increased from 85.40%to 94.87%.As the loading gradually increased,the hydrophilicity of the MMMs increased,significantly enhancing their fouling *** strongest anti-fouling ability observed was 94.74%,which was 2.02 times greater than that of the pure *** the same time,the MMMs contained internal amide and hydrogen bonds during the preparation process,forming a cross-linked structure,which further enhanced the mechanical strength and chemical *** summary,the MMMs with high retention rate,strong permeability,and anti-fouling ability were successfully prepared.

关键词： Poly(arylene ether ketone)-containing Carboxyl groups(PAEK-COOh) UiO-66-Nh_(2)@graphene oxide hydrophilic modification Ultra-high selectivity Strong anti-fouling

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Facile synthesis of hierarchical NaX zeolite from natural kaolinite for efficient Knoevenagel condensation

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Chinese journal of Chemical Engineering 2024年第1期65卷 75-84页

作者： Wen Xiao Peng dong Chan Wang jingdong Xu Tiesen Li haibo Zhu Tinghai Wang Renwei Xu Yuanyuan Yue National Engineering Research Center of Chemical Fertilizer Catalyst College of Chemical EngineeringFuzhou UniversityFuzhou 350108China Qingyuan Innovation Laboratory Quanzhou 362801China Sinochem Quanzhou Energy Technology Co. Ltd.Quanzhou 362000China

Zeolite catalysts have found extensive applications in the synthesis of various fine ***,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic ***,we explore an economic and environmentally friendly method for synthesizing hierarchical NaX zeolite that exhibits improved catalytic performance in the Knoevenagel condensation reaction for producing the useful fine chemical *** synthesis was achieved via a low-temperature activation of kaolinite and subsequent in-situ transformation strategy without any template or *** characterizations reveal that the synthesized NaX zeolite has both intercrystalline and intra-crystalline mesopores,smaller crystal size,and larger external specific surface area compared to commercial NaX *** mechanism investigations show that the inter-crystalline mesopores are generated by stacking smaller crystals formed from in-situ crystallization of the depolymerized kaolinite,and the intra-crystalline mesopores are inherited from the pores in the depolymerized *** synthesis strategy provides an energy-saving and effective way to construct hierarchical zeolites,which may gain wide applications in fine chemical manufacturing.

关键词： hierarchical NaX zeolite Template-free synthesis Natural kaolinite Knoevenagel condensation

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Electronic structure and spin state regulation of vanadium nitride via a sulfur doping strategy toward flexible zinc-air batteries

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journal of Energy Chemistry 2024年第2期89卷 239-249,I0007页

作者： Daijie Deng honghui Zhang jianchun Wu Xing Tang Min Ling Sihua dong Li Xu henan Li huaming Li Institute for Energy Research Institute of Quantum and Sustainable TechnologySchool of Chemistry and Chemical EngineeringSchool of Materials Science and EngineeringJiangsu Province and Education Ministry Co-Sponsored Synergistic Innovation Center of Modern Agricultural EquipmentJiangsu UniversityZhenjiang 212013JiangsuChina Key Laboratory of Radio Frequency and Micro-Nano Electronics of jiangsu Province Nanjing 210023JiangsuChina Zhenjiang Kangyuan Electrical Appliance Co. Ltd.Zhenjiang 212013JiangsuChina College of Chemical and Biological Engineering Zhejiang UniversityHangzhou 310027ZhejiangChina YTO Group Corporation dongfanghong(henan)Agricultural Service Technology Co. Ltd.Luoyang 471033HenanChina

Owing to the distinctive structural characteristics,vanadium nitride(VN)is highly regarded as a catalyst for oxygen reduction reaction(ORR)in zinc-air batteries(ZABs).however,VN exhibits limited intrinsic ORR activity due to the weak adsorption ability to O-containing ***,the S-doped VN anchored on N,S-doped multi-dimensional carbon(S-VN/Co/NS-MC)was constructed using the solvothermal and in-situ doping *** sulfur atoms into VN species alters the electron spin state of vanadium in the S-VN/Co/NS-MC for regulating the adsorption energy of vanadium sites to oxygen *** introduced sulfur atoms polarize the V 3d_(z)^(2) electrons,shifting spin-down electrons closer to the Fermi level in the S-VN/Co/***,the introduction of sulfur atoms into VN species enhances the adsorption energy of vanadium sites for oxygen ****OOh dissociation transitions from being unspontaneous on the VN surface to a spontaneous state on the S-doped VN ***,the ORR barrier on the S-VN/Co/NS-MC surface is *** S-VN/Co/NS-MC demonstrates a higher half-wave potential and limiting current density compared to the VN/Co/*** S-VN/Co/NS-MC-based liquid ZABs display a power density of 195.7 m W cm^(-2),a specific capacity of 815.7 m A h g^(-1),and a cycling stability exceeding 250 *** S-VN/Co/NS-MC-based flexible ZABs are successfully employed to charge both a smart watch and a mobile *** approach holds promise for advancing the commercial utilization of VN-based catalysts in ZABs.

关键词： S-doped VN Electronic structures Spin state regulation Oxygen reduction reaction Zinc-air batteries

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Two UV organic-inorganic hybrid antimony-based materials with superior optical performance derived from cation-anion synergetic interactions

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Chinese Chemical Letters 2024年第9期35卷 442-446页

作者： Pu Zhang Xiang Mao Xuehua dong Ling huang Liling Cao Daojiang Gao Guohong Zou College of Chemistry and Materials Science Sichuan Normal UniversityChengdu 610066China College of Chemistry Sichuan UniversityChengdu 610065China

Finding suitable strategies to effectively enhance the optical properties of materials are the goal being pursued by ***,cation-anion synergetic interactions strategy was proposed to develop two novel organic-inorganic hybrid antimony-based optical materials,(C_(3)h_(5)N_(2))Sb F_(2)SO_(4)(I)and(C_(5)h_(6)N)Sb F_(2)SO_(4)(Ⅱ),which were obtained by introducing Sb^(3+)cation containing stereochemically active lone-pair(SCALP)and organicπ-conjugated cations into sulphate *** synergistic interactions of the organicπ-conjugated cations,the inorganic[SbO_(2)F_(2)]^(3-)seesaw anions and the[SO_(4)]^(2-)distorted tetrahedra anions make their ultraviolet(UV)absorption edges approach 297 and 283 nm,respectively,and raise their birefringence up to 0.193@546 nm and 0.179@546 nm,***,although the two compounds have the same stoichiometric ratio and similar one-dimensional(1D)chain structure,they show opposite macroscopic symmetry,where the NCS compound(Ⅱ)exhibits a large secondharmonic generation(ShG)response(1.6 times that of Kh_(2)PO_(4)).The two reported compounds are found to be promising UV optical materials in the experimental tests.

关键词： Antimony-based crystals Cation-anion synergetic interactions Large birefringence Short UV absorption edge Organic-inorganic hybrid Ionothermal synthesis

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