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Chinese Journal of Chemical Engineering 2022年第3期35卷 353-359页

作者： Yachen Deng Shifu Wang Yanqiang Huang Xuning Li State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

MOF-based materials have been widely explored in electrochemical CO_(2)reduction reactions for the production of valuable chemicals.Understanding the reconstruction of those catalysts under working conditions is crucial for the identification of active sites and clarification of reaction mechanism.Herein,a series of six N coordinated Sn-based metal-organic frameworks(Sn-N6-MOFs)are newly developed for electrochemical CO_(2)reduction(CO_(2)RR).2%Sn-N6-MOF achieves the optimal catalytic performance with a formate Faradaic efficiency of~85%and a current density of 23 mA·cm^(-2) at-1.23 V vs.RHE.In-situ Raman results combined with ex-situ ^(119)Sn Mössbauer measurements reveal the structural reconstruction of Sn-N6-MOFs during CO_(2)RR,generating tin nanoclusters as the real active sites for CO_(2)electroreduction to HCOOH.

关键词： structural reconstruction Metal-organic frameworks Mössbauer spectroscopy Electrochemical CO_(2)reduction

Immobilization of Oxyanions on the Reconstructed Heterostructure Evolved from a Bimetallic Oxysulfide for the Promotion of Oxygen Evolution Reaction

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Nano-Micro Letters 2023年第10期15卷 547-564页

作者： Kai Yu Hongyuan Yang Hao Zhang Hui Huang Zhaowu Wang Zhenhui Kang Yang Liu Prashanth W.Menezes Ziliang Chen Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon‑Based Functional Materials and DevicesJoint International Research Laboratory of Carbon‑Based Functional Materials and DevicesSoochow UniversitySuzhou 215123People’s Republic of China Department of Chemistry:Metalorganics and Inorganic Materials Technical University of BerlinStrase Des 17 Juni 135.Sekr.C210623 BerlinGermany Materials Chemistry Group for Thin Film Catalysis–CatLab Helmholtz-Zentrum Berlin fur Materialien und EnergieAlbert‑Einstein‑Str.1512489 BerlinGermany School of Physics and Engineering Longmen LaboratoryHenan University of Science and TechnologyLuoyang 471023People’s Republic of China

Efficient and durable oxygen evolution reaction(OER)requires the electrocatalyst to bear abundant active sites,optimized electronic structure as well as robust component and mechanical stability.Herein,a bimetallic lanthanum-nickel oxysulfide with rich oxygen vacancies based on the La_(2)O_(2)S prototype is fabricated as a binder-free precatalyst for alkaline OER.The combination of advanced in situ and ex situ characterizations with theoretical calculation uncovers the synergistic effect among La,Ni,O,and S species during OER,which assures the adsorption and stabilization of the oxyanion SO_(4)^(2-)onto the surface of the deeply reconstructed porous heterostructure composed of confining Ni OOH nanodomains by La(OH)_3 barrier.Such coupling,confinement,porosity and immobilization enable notable improvement in active site accessibility,phase stability,mass diffusion capability and the intrinsic Gibbs free energy of oxygen-containing intermediates.The optimized electrocatalyst delivers exceptional alkaline OER activity and durability,outperforming most of the Ni-based benchmark OER electrocatalysts.

关键词： Lanthanum-nickel oxysulfide Rare earth metal Immobilization of oxyanions structural reconstruction Oxygen evolution catalysis

Dual‑Doped Nickel Sulfide for Electro‑Upgrading Polyethylene Terephthalate into Valuable Chemicals and Hydrogen Fuel

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纳微快报:英文版 2023年第11期15卷 385-399页

作者： Zhijie Chen Renji Zheng Teng Bao Tianyi Ma Wei Wei Yansong Shen Bing‑Jie Ni Centre for Technology in Water and Wastewater School of Civil and Environmental EngineeringUniversity of Technology SydneySydneyNSW 2007Australia School of Minerals Processing and Bioengineering Central South UniversityChangsha 410083People’s Republic of China School of Biology Food and Environment EngineeringHefei UniversityHefei 230601People’s Republic of China School of Science STEM CollegeRMIT UniversityMelbourneVIC 3000Australia School of Chemical Engineering University of New South WalesSydneyNSW 2052Australia

Electro-upcycling of plastic waste into value-added chemicals/fuels is an attractive and sustainable way for plastic waste management.Recently,electrocatalytically converting polyethylene terephthalate(PET)into formate and hydrogen has aroused great interest,while developing low-cost catalysts with high efficiency and selectivity for the central ethylene glycol(PET monomer)oxidation reaction(EGOR)remains a challenge.Herein,a high-performance nickel sulfide catalyst for plastic waste electro-upcycling is designed by a cobalt and chloride co-doping strategy.Benefiting from the interconnected ultrathin nanosheet architecture,dual dopants induced upshifting d band centre and facilitated in situ structural reconstruction,the Co and Cl co-doped Ni_(3)S_(2)(Co,Cl-NiS)outperforms the singledoped and undoped analogues for EGOR.The self-evolved sulfide@oxyhydroxide heterostructure catalyzes EG-to-formate conversion with high Faradic efficiency(>92%)and selectivity(>91%)at high current densities(>400 mA cm^(−2)).Besides producing formate,the bifunctional Co,Cl-NiS-assisted PET hydrolysate electrolyzer can achieve a high hydrogen production rate of 50.26 mmol h^(−1)in 2 M KOH,at 1.7 V.This study not only demonstrates a dual-doping strategy to engineer cost-effective bifunctional catalysts for electrochemical conversion processes,but also provides a green and sustainable way for plastic waste upcycling and simultaneous energy-saving hydrogen production.

关键词： Hydrogen energy Electro-upcycling structural reconstruction Organic waste upcycling d Band centre

Recent advances in metal-organic frameworks for oxygen evolution reaction electrocatalysts

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中国科学:化学英文版 2023年第10期66卷 2754-2779页

作者： Ming Liu Yin-Qiang Zhang Xuemin Wang Feifan Lang Na Li Xian-He Bu School of Materials Science and Engineering Nankai UniversityTianjin 300350China State Key Laboratory of Elemento-Organic Chemistry College of ChemistryNankai UniversityTianjin 300071China

The anodic oxygen evolution reaction(OER)can be combined with various cathodic reactions to enable the electrochemical synthesis of diverse chemicals and fuels,particularly in water electrolysis for hydrogen production.It is however exhibiting a high overpotential due to the sluggish four-electron transfer process,which is considered the decisive reaction in energy conversion systems.In recent years,metal-organic frameworks(MOFs)have emerged as the ideal catalysts for accelerating OER.This is primarily because of their orderly porous architecture,structural tailorability,and compositional diversity.This review systematically summarizes the recent research progress in pristine MOF electrocatalysts for OER,which covers the construction strategies and electrocatalytic performance of more than eight types of MOFs.Additionally,the partial/complete structural reconstructions and their effects on MOF-based OER electrocatalysts are highlighted.In particular,the development process of“discovery,explanation,and utilization”for the structural reconstructions of MOF electrocatalysts is outlined.Furthermore,the catalytic mechanisms are elaborated in detail,aiming to provide insight into the rational design and performance optimization of MOF-based OER electrocatalysts.The challenges and future perspectives of MOF-based OER electrocatalysts for industrial applications are also discussed.

关键词： metal-organic frameworks electrocatalysts oxygen evolution reaction structural reconstruction active sites

Simultaneously mastering operando strain and reconstruction effects via phase-segregation strategy for enhanced oxygen-evolving electrocatalysis

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Journal of Energy Chemistry 2023年第7期82卷 572-580,I0012页

作者： Daqin Guan Chenliang Shi Hengyue Xu Yuxing Gu Jian Zhong Yuchen Sha Zhiwei Hu Meng Ni Zongping Shao State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211800JiangsuChina Department of Building and Real Estate Research Institute for Sustainable Urban Development(RISUD)and Research Institute for Smart Energy(RISE)The Hong Kong Polytechnic UniversityHung HomKowloon 999077Hong KongChina Institute of Biopharmaceutical and Health Engineering Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055GuangdongChina Max-Planck-Institute for Chemical Physics of Solids Nöthnitzer Str.40Dresden 01187Germany WA School of Mines:Minerals Energy and Chemical EngineeringCurtin UniversityPerthWestern Australia 6845Australia

Material strain and reconstruction effects are critical for catalysis reactions,but current insights into operando strain effects during reaction and means to master catalyst reconstruction are still lacking.Here,we propose a facile thermal-induced phase-segregation strategy to simultaneously master material operando strain and reconstruction effects for enhanced oxygen-evolving reaction(OER).Specifically,self-assembled and controllable layered LiCoO_(2)phase and Co_(3)O_(4)spinel can be generated from pristine Li2Co_(2)O_(4)spinel via Li and O volatilization under different temperatures,realizing controllable proportions of two phases by calcination temperature.Combined operando and ex-situ characterizations reveal that obvious tensile strain along(003)plane appears on layered LixCoO_(2)phase during OER,while low-valence Co_(3)O_(4)phase transforms into high-valence CoOOHx,realizing simultaneous operando strain and reconstruction effects.Further experimental and computational investigations demonstrate that both strained LixCoO_(2)phase and reconstructed CoOOHxcompound contribute to the beneficial adsorption of important OH-reactants,while respective roles in activity and stability are uncovered by exploring their latticeoxygen participation mechanism.This work not only reveals material operando strain effects during OER,but also inaugurates a new thermal-induced phase-segregation strategy to artificially master material operando strain and reconstruction effects,which will enlighten rational material design for many potential reactions and applications.

关键词： Operando strain structural reconstruction Phase-segregation strategy Operando synergistic effects Oxygen-evolving reaction

Deciphering of advantageous electrocatalytic water oxidation behavior of metal-organic framework in alkaline media

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Nano Research 2021年第12期14卷 4680-4688页

作者： Ming Liu Lingjun Kong Xuemin Wang Jie He Jijie Zhang Jian Zhu Xian-He Bu School of Materials Science and Engineering National Institute for Advanced MaterialsTKL of Metal and Molecule Based Material ChemistryNankai UniversityTianjin300350China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin300071China

Carboxylic acid-based metal-organic frameworks(MOFs)are normally passed for the“pre-catalysts”for oxygen evolution reaction(OER)due to the hydroxides constructed in-situ during its alkaline hydrolysis process(AHP)in lye.Whereas,it remains a mystery that they show advantageous activity over prototypical hydroxides when they are directly acted as OER catalysts.Herein,we propose for the first time that the steric hindrance effect of Nafion can induce enhanced catalytic activity of such MOFs.Different from conventional catalysts without AHP,the Nafion with 3D structure weakens the AHP of Co-MOF nanoribbons,thus forming small size and low crystallinity species(cobalt hydroxide)with more active sites.And the existence of Nafion also optimizes its electronic structure,which is confirmed by transmission electron microscopy(TEM),in-situ UV absorption spectra,in-situ Raman spectroscopy and so on.Compared with Co-MOF-K obtained by directly immersing the Co-MOF nanoribbons in 1.0 M KOH,the Co-MOF-NK obtained by AHP of Co-MOF mixed with Nafion shows better catalytic activity.Based on the above inspiration,we realized the low overpotential of 268 mV at 10 mA·cm^(−2) by preparing CoFe-MOF-NK.This work provides a new understanding of the structural reconstruction of MOFs in the field of electrocatalysis.

关键词： metal-organic frameworks structural reconstruction Nafion stereo hindrance water oxidation

Rational construction of metal–base synergetic sites on Au/Mg-beta catalyst for selective aerobic oxidation of 5-hydroxymethylfurfural

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Journal of Energy Chemistry 2021年第11期30卷 599-609,I0014页

作者： Zhiguo Zhu Xiongjie Gao Xiuming Wang Mengdie Yin Qingyao Wang Wanzhong Ren Bo Wang Hongying Lü Weiping Liao College of Chemistry and Chemical Engineering Yantai University30 Qingquan RoadYantai 264005ShandongChina Library Yantai University30 Qingquan RoadYantai 264005ShandongChina Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology School of Chemistry and Chemical EngineeringLiaocheng UniversityLiaocheng 252059ShandongChina

The selective aerobic oxidation of biomass-derived 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid (FDCA, a potential renewable substitution of fossil-based terephthalic acid to produce polyethylene 2,5-furandicarboxylate plastic) is an appealing transformation for constructing eco-friendly and sustainable chemical processes. Au supported catalysts have showed encouraging performances for this well-received conversion, whose catalytic behavior was greatly affected by the adopted support derived from the existence of metal-support interactions. Herein, a series of Mg-Beta zeolites were hydrothermally synthesized via developed structural reconstruction, which were employed as basic supports for Au catalysts to construct bifunctional catalysts. The relationship between structure (Au particle size, basicity within zeolites and Auδ+ contents) and FDCA yield was concretely established. The conclusion was made that the utilization of Mg-Beta zeolites with strong basicity as the support could not only improve the FDCA yield but also decrease the amount of additional base. Furthermore, the possible reaction mechanism was also proposed via tracking time-dependent variations of corresponding organics and controlled experiment. This work provides some guidance for rationally designing multifunctional catalysts in the view of integrating metal catalysts with metallosilicate zeolites, which was beneficial to the catalytic upgrading of organic compounds with multiple functional groups.

关键词： 5-Hydroxymethylfurfural Aerobic oxidation 2,5-Furandicarboxylic acid Bifunctional Au/Mg-Beta catalyst structural reconstruction