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Accelerating Oxygen Electrocatalysis Kinetics on Metal-Organic Frameworks via Bond Length Optimization

Nano-Micro Letters 2024年第9期16卷 279-290页

作者： Fan He Yingnan Liu Xiaoxuan Yang Yaqi Chen Cheng‑Chieh Yang Chung‑Li Dong Qinggang He Bin Yang Zhongjian Li Yongbo Kuang lecheng lei Liming Dai Yang Hou Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China Institute of Zhejiang University-Quzhou Quzhou 324000People’s Republic of China Ningbo Institute of Materials Technology and Engineering Chinese Academy of SciencesNingbo 315201People’s Republic of China School of Biological and Chemical Engineering NingboTech UniversityNingbo 315100People’s Republic of China Department of Physics Tamkang UniversityNew Taipei 25137TaiwanPeople’s Republic of China Australian Carbon Materials Centre(A‑CMC) School of Chemical EngineeringUniversity of New South WalesSydneyNSW 2051Australia

Metal-organic frameworks(MOFs)have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity,but the limited catalytic activity and stability has hampered their practical use in water splitting.Herein,we develop a bond length adjustment strategy for optimizing naphthalene-based MOFs that synthesized by acid etching Co-naphthalenedicarboxylic acid-based MOFs(donated as AE-CoNDA)to serve as efficient catalyst for water splitting.AE-CoNDA exhibits a low overpotential of 260 mV to reach 10 mA cm^(−2)and a small Tafel slope of 62 mV dec^(−1)with excellent stability over 100 h.After integrated AE-CoNDA onto BiVO_(4),photocurrent density of 4.3 mA cm^(−2)is achieved at 1.23 V.Experimental investigations demonstrate that the stretched Co-O bond length was found to optimize the orbitals hybridization of Co 3d and O 2p,which accounts for the fast kinetics and high activity.Theoretical calculations reveal that the stretched Co-O bond length strengthens the adsorption of oxygen-contained intermediates at the Co active sites for highly efficient water splitting.

关键词： Metal-organic frameworks Bond length adjustment Spin state transition Orbitals hybridization Water splitting

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A one-pot process based on P_(44414)Cl-HCl aqueous biphasic system for recovering rare earth elements from NdFeB permanent magnet

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Chinese Chemical Letters 2022年第2期33卷 953-956页

作者： Chuanying Liu Qibin Yan Xingwang Zhang lecheng lei Chengliang Xiao College of Chemical and Biological Engineering Zhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China

Recovering critical metals from secondary resources have attracted great interest recently.In this work,a green one-pot leaching-extraction process based on tributyl(tetradecyl)phosphonium chloride (P_(44414)Cl)aqueous biphasic system (ABS) was developed to efficiently recover rare earth elements (REEs) from Nd Fe B permanent magnet.The reaction process,phase separation mechanism,and operation conditions were thoroughly investigated.It is found that the P_(44414)Cl-HCl ABS showed strong extraction ability towards Fe (>99%) whereas only a few REEs (<10%) were extracted,leading to extremely high separation selectivity between Fe and REEs.The characterization results showed that the coordination differences of Fe and Nd in HCl were the main driving forces for such highly selective separation.The phase diagram of P_(44414)Cl-Nd Cl_(3)ABS indicated that the salting-out effect of Nd Cl_(3)was stronger than common chlorides.Due to the hydrophobic property of P_(44414)[Fe Cl_(4)]and salting-out effect of Nd Cl_(3),the P_(44414)Cl could directly form ABS at room temperature after dissolving practical roasted Nd Fe B samples without any other operations and reagents.REEs and Fe could be mutually separated in just one step.Compared with traditional liquid-liquid extraction or ABS separation,this recovery process is green and facile and shows great application prospects in the field of rare-earth recovery.

关键词： Rare earth Ionic liquid NdFeB permanent magnet P_(44414)Cl Aqueous biphasic system

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Co anchored on porphyrinic triazine-based frameworks with excellent biocompatibility for conversion of CO_(2)in H_(2)-mediated microbial electrosynthesis

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Frontiers of Chemical Science and Engineering 2022年第12期16卷 1761-1771页

作者： Folin Liu Shaohua Feng Siyuan Xiu Bin Yang Yang Hou lecheng lei Zhongjian Li College of Chemical and Biological Engineering Key Laboratory of Biomass Chemical Engineering of Ministry of EducationZhejiang UniversityHangzhou 310027China Institute of Zhejiang University—Quzhou Quzhou 324000China Academy of Ecological Civilization Zhejiang UniversityHangzhou 310027China

Microbial electrosynthesis is a promising alternative to directly convert CO_(2)into long-chain compounds by coupling inorganic electrocatalysis with biosynthetic systems.However,problems arose that the conventional electrocatalysts for hydrogen evolution may produce extensive by-products of reactive oxygen species and cause severe metal leaching,both of which induce strong toxicity toward microorganisms.Moreover,poor stability of electrocatalysts cannot be qualified for long-term operation.These problems may result in poor biocompatibility between electrocatalysts and microorganisms.To solve the bottleneck problem,Co anchored on porphyrinic triazine-based frameworks was synthesized as the electrocatalyst for hydrogen evolution and further coupled with Cupriavidus necator H16.It showed high selectivity for a four-electron pathway of oxygen reduction reaction and low production of reactive oxygen species,owing to the synergistic effect of Co–Nx modulating the charge distribution and adsorption energy of intermediates.Additionally,low metal leaching and excellent stability were observed,which may be attributed to low content of Co and the stabilizing effect of metalloporphyrins.Hence,the electrocatalyst exhibited excellent biocompatibility.Finally,the microbial electrosynthesis system equipped with the electrocatalyst successfully converted CO_(2)to poly-β-hydroxybutyrate.This work drew up a novel strategy for enhancing the biocompatibility of electrocatalysts in microbial electrosynthesis system.

关键词： microbial electrosynthesis hydrogen evolution reaction metalloporphyrins biocompatibility CO_(2)conversion

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Spin polarization strategy to deploy proton resource over atomic-level metal sites for highly selective CO_(2) electrolysis

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Frontiers of Chemical Science and Engineering 2022年第12期16卷 1772-1781页

作者： Yingjie Zhao Xinyue Wang Xiahan Sang Sixing Zheng Bin Yang lecheng lei Yang Hou Zhongjian Li Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China Nanostructure Research Centre Wuhan University of TechnologyWuhan 430070China

Unlocking of the extremely inert C=O bond during electrochemical CO_(2) reduction demands subtle regulation on a key“resource”,protons,necessary for intermediate conversion but also readily trapped in water splitting,which is still challenging for developing efficient single-atom catalysts limited by their structural simplicity usually incompetent to handle this task.Incorporation of extra functional units should be viable.Herein,a proton deployment strategy is demonstrated via“atomic and nanostructured iron(A/N-Fe)pairs”,comprising atomically dispersed iron active centers spin-polarized by nanostructured iron carbide ferromagnets,to boost the critical protonation steps.The as-designed catalyst displays a broad window(300 mV)for CO selectivity>90%(98%maximum),even outperforming numerous cutting-edge M–N–C systems.The well-placed control of proton dynamics by A/N-Fe can promote*COOH/*CO formation and simultaneously suppress H2 evolution,benefiting from the magnetic-proximity-induced exchange splitting(spin polarization)that properly adjusts energy levels of the Fe sites’d-shells,and further those of the adsorbed intermediates’antibonding molecular orbitals.

关键词： CO_(2)electrolysis/single-atom catalysts/spin polarization/proton dynamics/in situ IR spectroscopy/kinetic isotope effect

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Ultrasmall Pt_(2)Sr alloy nanoparticles as efficient bifunctional electrocatalysts for oxygen reduction and hydrogen evolution in acidic media

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Journal of Energy Chemistry 2022年第1期31卷 315-322,I0009页

作者： Xiangnan Liu Shaoyun Hao Guokui Zheng Zhiwei Su Yahui Wang Qiqi Wang lecheng lei Yi He Xingwang Zhang Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological Engineering Zhejiang UniversityHangzhou 310027ZhejiangChina Institute of Zhejiang University-Quzhou Quzhou 324000ZhejiangChina

Electrocatalytic oxygen reduction reaction(ORR)and hydrogen evolution reaction(HER)in acidic media are vital for the applications of renewable energy electrolyzers.However,the low mass activity of noble Pt urgently needs to be improved due to the strong binding energetics of oxygen species(*O)with Pt sites.Here we report fine PtxSr alloy(-2 nm)supported on N-doped carb on(NC)pyrolyzing from ZIF-8 as bifunctional electrocatalysts toward ORR and HER in acidic media.The representative Pt_(2)Sr/NC exhibits an onset potential of 0.94 V vs.RHE and half-wave potential of 0.84 V toward ORR,and a low over-potential of 27 mV(10 mA cm^(-2))toward HER,respectively.Significantly,the mass activities of Pt_(2)Sr/NC are 6.2 and 2.6 times higher than that of Pt/C toward ORR(at 0.9 V)and HER(at-30 mV),respectively.Simultaneously,Pt_(2)Sr/NC possesses a retention rate of 90.97%toward acidic ORR after 35000 s of continuous operation.Through density functional theory(DFT)calculations and X-ray photoelectron spectroscopy analysis,the incorporation of Sr into Pt forming Pt_(2)Sr alloy redistributes the electronic structures of Pt-Pt bonds,changing the rate-determining step for the ORR on Pt sites from the formation of*OH from*O to the generation of*OOH along with decreasing the energy barrier,which is also confirmed by the downshift of d band center.Meanwhile,the downshift of d band center also leads to the optimization of the adsorption energy(H*)with Pt,significantly improving Pt_(2)Sr/NC toward HER.

关键词： Acidic media Alloy Oxygen reduction reaction Hydrogen evolution reaction Density functional theory

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Rational design on photoelectrodes and devices to boost photoelectrochemical performance of solar-driven water splitting: a mini review

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Frontiers of Chemical Science and Engineering 2022年第6期16卷 777-798页

作者： Siliu Lyu Muhammad Adnan Younis Zhibin Liu Libin Zeng Xianyun Peng Bin Yang Zhongjian Li lecheng lei Yang Hou Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China

As an eco-friendly,efficient,and low-cost technique,photoelectrochemical water splitting has attracted growing interest in the production of clean and sustainable hydrogen by the conversion of abundant solar energy.In the photoelectrochemical system,the photoelectrode plays a vital role in absorbing the energy of sunlight to trigger the water splitting process and the overall efficiency depends largely on the integration and design of photoelectrochemical devices.In recent years,the optimization of photoelectrodes and photoelectrochemical devices to achieve highly efficient hydrogen production has been extensively investigated.In this paper,a concise review of recent advances in the modification of nanostructured photoelectrodes and the design of photoelectrochemical devices is presented.Meanwhile,the general principles of structural and morphological factors in altering the photoelectrochemical performance of photoelectrodes are discussed.Furthermore,the performance indicators and first principles to describe the behaviors of charge carriers are analyzed,which will be of profound guiding significance to increasing the overall efficiency of the photoelectrochemical water splitting system.Finally,current challenges and prospects for an in-depth understanding of reaction mechanisms using advanced characterization technologies and potential strategies for developing novel photoelectrodes and advanced photoelectrochemical water splitting devices are demonstrated.

关键词： photoelectrochemical water splitting photoelectrodes hydrogen production charge separation catalytic mechanism

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Optimizing electronic structure of NiFe LDH with Mn-doping and Fe_(0.64)Ni_(0.36)alloy for alkaline water oxidation under industrial current density

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Nano Research 2023年第7期16卷 8953-8960页

作者： Yang Qian Fan Zhang Lingshu Qiu Weiwei Han Zixu Zeng lecheng lei Yi He Ping Li Xingwang Zhang Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China

Alkaline electrolyzers for water splitting under the industrial current densities are always burdened with huge energy consumption due to the high overpotential and poor stability of the anode nanocatalysts for oxygen evolution reaction(OER).Inspired by the interfacial charge transfer for enhancing the performance,a series of in-situ grown interfacial Mn-NiFe lactate dehydrogenase(LDH)was designed on the Fe_(0.64)Ni_(0.36)/NM(nickel mesh)alloy layer.The optimized Mn_(0.15)-NiFe LDH/Fe_(0.64)Ni_(0.36)/NM exhibited an ultralow overpotential of 295 mV to drive 500 mA·cm^(-2)and an incredible stability under large current density.The interfacial space and heteroatom doping synergistically triggered the electronic structure optimization to promote electron transfer and ensure the durability of the high-current reaction.Notably,the designed Mn_(0.15)-NiFe LDH/Fe_(0.64)Ni_(0.36)/NM as an anode in an integral alkaline electrolyzer exhibited a cell voltage of 1.78 V at 500 mA·cm^(-2) with a stability of 366 h.Density functional theory(DFT)calculations further demonstrated the synergistic effect of alloy layer introduction and Mn doping could accelerate electron transfer and stabilize the charged active center to activate the NiFe LDH and reduce the OER energy barrier.Our work offers new insights into developing efficient self-supported catalysts for high-current alkaline water oxidation.

关键词： heteroatom doping alloy layer introduction synergistic effect high-current alkaline water oxidation

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Layered bismuth oxide/bismuth sulfide supported on carrageenan derived carbon for efficient carbon dioxide electroreduction to formate

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Chinese Journal of Chemical Engineering 2022年第3期35卷 116-123页

作者： Xiangzhao Hu Junjie Sun Wanzhen Zheng Sixing Zheng Yu Xie Xiang Gao Bin Yang Zhongjian Li lecheng lei Yang Hou Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China Department of Material Chemistry Nanchang Hangkong UniversityNanchang 330063China School of Biological and Chemical Engineering Ningbo Technology UniversityNingbo 315100China

Electrochemical reduction of carbon dioxide(CO_(2)ER)into formate plays a crucial role in CO_(2)conversion and utilization.However,it still faces the problems of high overpotential and poor catalytic stability.Herein,we report a hybrid CO_(2)ER electrocatalyst composed of layered bismuth sulfide(Bi_(2)S_(3))and bismuth oxide(Bi_(2)O_(3))supported on carrageenan derived carbon(Bi-CDC)prepared by a combined pyrolysis with hydrothermal treatment.In such 3 D hybrid,layered Bi_(2)O_(3)and Bi_(2)S_(3)are uniformly grown on nanocarbon supports.Benefiting from strong synergistic effect between Bi_(2)O_(3)/Bi_(2)S_(3)and nanocarbon,Bi-CDC-1:2 displays a high Faradic efficiency(FE)of>80%for formate production in the range of-0.9 V to-1.1 V with the maximum formate FE of 85.6%and current density of 14.1 mA·cm^(-2) at-1.0 V.Further,a positive onset potential of-0.5 V,a low Tafel slope of 112.38 mV·dec^(-1),and a slight performance loss during long-term CO_(2)ER tests are observed on Bi-CDC-1:2.Experimental results shows that the better CO_(2)ER performance of Bi-CDC-1:2 than that of Bi_(2)O_(3)can be attributed to the strong interfacial interactions between nanocarbons and Bi_(2)O_(3)/Bi_(2)S_(3).In situ ATR-FTIR measurements reveal that the rate-determining step in the CO_(2)ER is the formation of HCOO^(*) intermediated.Compared with carbon support,Bi-CDC-1:2 can promote the production of HCOO^(*) intermediate and thus promoting CO_(2)ER kinetic.

关键词： Nanomaterials Catalyst Selectivity Bi_(2)S_(3)/Bi_(2)O_(3) CO_(2)electroreduction Formate

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Enhanced hydrogen evolution from the face-sharing[RuO6]octahedral motif

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Journal of Energy Chemistry 2021年第5期30卷 276-282页

作者： Fan Zhang Shaoyun Hao Guokui Zheng lecheng lei Xingwang Zhang Key Laboratory of Biomass Chemical Engineering of Ministry of Education Department of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina Institute of Zhejiang University-Quzhou Quzhou 324000ZhejiangChina

Hampered by the ambiguous mechanism of hydrogen evolution reaction(HER)in basic media,the exploration of highly efficient catalytically active sites for alkaline HER is of significance.Herein,a metal oxide Sr_(4)Ru_(2)O_(9)engineering a face-sharing[RuO_(6)]octahedra motif was synthesized through the solid-state method,and served as HER electrocatalyst.Benefited from the Ru-Ru metallic bonding crossing the common plane,the H*adsorption and reaction energy barriers were optimized.Sr_(4)Ru_(2)O_(9)only required an ultra-small overpotential(η10)of 28 m V at a current density of 10 mA cm^(-2) for HER in 1.0 M KOH with an exceptional stability(180 hours),outperforming the commercial Pt/C(η10=38 mV).These findings suggest a fresh insight in designing novel active sites for electrocatalysis.

关键词： Catalytically active site Face-sharing octahedra Electrocatalysis Hydrogen evolution reaction

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Application of in-plasma catalysis and post-plasma catalysis for methane partial oxidation to methanol over a Fe_2O_3-CuO/γ-Al_2O_3 catalyst

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Journal of Natural Gas Chemistry 2010年第6期19卷 628-637页

作者： Lin Chen Xingwang Zhang Liang Huang lecheng lei Institute of Industrial Ecology and Environment Zhejiang University Hangzhou 310027 Zhejiang China Institute of Environmental Science and Engineering College of Materials and Environmental Engineering Hangzhou Dianzi University Hangzhou 310018 Zhejiang China

Methane partial oxidation to methanol （MPOM） using dielectric barrier discharge over a Fe2O3-CuO/γ-Al2O3 catalyst was performed.The multicomponent catalyst was combined with plasma in two different configurations,i.e.,in-plasma catalysis （IPC） and post-plasma catalysis （PPC）.It was found that the catalytic performance of the catalysts for MPOM was strongly dependent on the hybrid configuration.A better synergistic performance of plasma and catalysis was achieved in the IPC configuration,but the catalysts packed in the discharge zone showed lower stability than those connected to the discharge zone in sequence.Active species,such as ozone,atomic oxygen and methyl radicals,were produced from the plasma-catalysis process,and made a major contribution to methanol synthesis.These active species were identified by the means of in situ optical emission spectra,ozone measurement and FT-IR spectra.It was confirmed that the amount of active species in the IPC system was greater than that in the PPC system.The results of TG,XRD,and N2 adsorption-desorption revealed that carbon deposition on the spent catalyst surface was responsible for the catalyst deactivation in the IPC configuration.

关键词： methane partial oxidation to methanol plasma catalysis combination synergistic performance catalytic stability

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