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Influence of Hydrogen Bonds between Solution Molecules on the Stability of Metal Cluster in Mass Spectrometry

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Chinese Journal of Structural chemistry 2022年

Electrospray ionization time-of-flight mass spectrometry （ESI-TOF-MS） has been recognized as a powerful technique for studying metal clusters’ chemical composition and reaction mechanisms. It is a great challenge in MS analysis to maintain the metal cluster molecules intact without fragmentation, which was achieved in this work by using mixed solvents to change the interaction between cluster molecules and solvent molecules, further affecting the fragmentation behaviors of the metal cluster in MS. Theoretical analysis reveals that the stability of the [（C）Au;Ag;(C;H;ONP);];cluster in ESI-TOF-MS is related to the strength of the chemical bonds between its own atoms and the bonding between the solvent and the cluster molecules.

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Rational design of three-dimensional branched NiCo-P@CoNiMo-P core/shell nanowire heterostructures for high-performance hybrid supercapacitor

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Journal of Energy chemistry 2021年第10期30卷 489-496,I0013页

作者： Yijing Huang Chong Luo Qiaobao Zhang Hehe Zhang Ming-Sheng Wang State Key Lab of Physical Chemistry of Solid Surfaces College of MaterialsXiamen UniversityXiamen 361005FujianChina

Owing to the dramatically enhanced charge-mass transport and abundant electrochemically active sites,transition metal compound electrodes are increasingly attractive for achieving high-performance supercapacitors(SCs).Here,we report the fabrication of nickel foam supported three-dimensional(3 D)branched nickel-cobalt phosphides@tri-metal cobalt-nickel-molybdenum phosphides core/shell nanowire heterostructures(denoted as NiCo-P@CoNiMo-P)as high-performance electrode materials for hybrid supercapacitors.The presence of multiple valences of the cations in such NiCo-P@CoNiMo-P enables rich redox reactions and promoted synergy effects.Benefiting from their collective effects,the resulting electrode demonstrates high specific capacity of 1366 C g^(-1) at 2 A g^(-1)(2.03 C cm^(-2) at2 mA cm^(-2))and 922 C g^(-1) at 10 A g^(-1),as well as good cycling stability(retaining~94%of the initial capacity after 6000 cycles at 15 A g^(-1)).A hybrid SC using the NiCo-P@CoNiMo-P as the positive electrode and N-doped rGOs as the negative electrode exhibits a high energy density of 81.4 Wh kg^(-1) at a power density of 1213 W kg^(-1) and a capacity retention of 132%even after 6000 cycles at 10 A g^(-1).Our findings can facilitate the material design for boosting the performance of transition metal compounds based materials for fast energy storage.

关键词： Transition metal phosphides Branched nanowire heterostructures Electrode materials Hybird supercapacitors

Ultrathin oxygen-containing graphdiyne wrapping CoP for enhanced electrocatalytic hydrogen generation

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Nano Research 2023年第4期16卷 5073-5079页

作者： Yan Lv Xueyan Wu Hao Li Hongbo Zhang Jiaxin Li Zhiyou Zhou Jixi Guo Dianzeng Jia state key laboratory of chemistry and Utilization of Carbon Based Energy Resources College of ChemistryXinjiang UniversityUrumqi830017China state key laboratory of physical chemistry of solid surfaces Xiamen UniversityXiamen 361005China

Graphdiyne(GDY)is fascinating in the construction of efficient and stable catalysts,but their performance is still somewhat restricted due to GDY’s thicker layers,as well as hydrophobic and relatively chemically inert surfaces.Herein,via oxidationexfoliation-reduction strategy,the self-supported electrode material of CoP nanosheets with ultrathin oxygen-containing GDY wrapping(CoP@RGDYO)for effective HER is constructed.The wrapping of ultrathin oxygen-containing GDY promotes charge transfer,improves the surface property,and enhances the acid and alkali resistance as well as the structural stability of the catalyst.As a result,CoP@RGDYO shows enhanced activity and stability in both acidic and alkaline media.Especially,it exhibits a low overpotential of 86 mV and exceptional stability under a 14000-cycle cyclic voltammetry scanning in alkaline media.This work provides new ideas for the design of GDY hybrid materials and the preparation of high-efficiency catalysts.

关键词： graphdiyne chainmail catalyst hydrophilicity stability hydrogen generation

Synergistic coupling of amorphous carbon and graphitic domains toward high-rate and long-life K^(+) storage

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Journal of Energy chemistry 2022年第10期31卷 533-541,I0013页

作者： Hehe Zhang Wangqin Li Jianhai Pan Zhefei Sun Bensheng Xiao Weibin Ye Chengzhi Ke Haowen Gao Yong Cheng Qiaobao Zhang Ming-Sheng Wang state key laboratory of physical chemistry of solid surfaces College of MaterialsXiamen UniversityXiamen 361005FujianChina Fujian key laboratory of surface and Interface Engineering for High Performance Materials(Xiamen University) Xiamen 361005FujianChina

Amorphous carbon materials hold great potential for practical use in potassium-ion batteries(PIBs)due to their abundant resources,low cost and high structural stability.However,given the challenge of sluggish potassiation kinetics,the rate performance of amorphous carbon is severely hindered.Herein,amorphous carbon compounded with graphitic domains(HG-CNTs)was proposed as an advanced anode for PIBs.As directly verified by in situ transmission electron microscopy(TEM),the graphitic domains guarantee fast K-ions transport in the carbon composite at a high current density,while the amorphous carbon shells ensure the structural integrity during potassiation,thus boosting its fast and durable K^(+)storage.As a PlB anode,the HG-CNTs electrode exhibits not only a super-stable long-term cyclability(191.6 mAh g^(-1)at 1 A g^(-1)with almost no capacity decay over 3000 cycles),but also an outstanding rate performance(184.5 mAh g^(-1)at 2 A g^(-1)).Ex situ Raman and TEM results further suggest that the highly reversible structure of HG-CNTs is responsible for its superior electrochemical stability.This work provides helpful insights into the development of carbonaceous electrodes with both high rate capability and long cycle life for PIBs.

关键词： Potassium-ion batteries Amorphous carbon Graphitic domains Synergistic effect In situ TEM

Integration of bio-inspired lanthanide-transition metal cluster and P-doped carbon nitride for efficient photocatalytic overall water splitting

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National Science Review 2021年第9期8卷 41-49页

作者： Rong Chen Gui-Lin Zhuang Zhi-Ye Wang Yi-Jing Gao Zhe Li Cheng Wang Yang Zhou Ming-Hao Du Suyuan Zeng La-Sheng Long Xiang-Jian Kong Lan-Sun Zheng Collaborative Innovation Center of chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surface and Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University College of Chemical Engineering Zhejiang University of Technology College of chemistry and Chemical Engineering Liaocheng University

Photosynthesis in nature uses the Mn4CaO5cluster as the oxygen-evolving center to catalyze the water oxidation efficiently in photosystem II. Herein, we demonstrate bio-inspired heterometallic Ln Co3(Ln=Nd, Eu and Ce) clusters, which can be viewed as synthetic analogs of the Ca Mn4O5cluster.Anchoring Ln Co3on phosphorus-doped graphitic carbon nitrides (PCN) shows efficient overall water splitting without any sacrificial reagents. The Nd Co3/PCN-c photocatalyst exhibits excellent water splitting activity and a quantum efficiency of 2.0%at 350 nm. Ultrafast transient absorption spectroscopy revealed the transfer of a photoexcited electron and hole into the PCN and Ln Co3for hydrogen and oxygen evolution reactions, respectively. A density functional theory (DFT) calculation showed the cooperative water activation on lanthanide and O-O bond formation on transition metal for water oxidation. This work not only prepares a synthetic model of a bio-inspired oxygen-evolving center but also provides an effective strategy to realize light-driven overall water splitting.

关键词： bio-inspired lanthanide-transition metal cluster photocatalytic overall water splitting synergistic effects oxygen-evolving center

Engineering Two-Phase Bifunctional Oxygen Electrocatalysts with Tunable and Synergetic Components for Flexible Zn-Air Batteries

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Nano-Micro Letters 2021年第8期13卷 175-190页

作者： Yanli Niu Xue Teng Shuaiqi Gong Mingze Xu Shi-Gang Sun Zuofeng Chen Shanghai key laboratory of Chemical Assessment and Sustainability School of Chemical Science and EngineeringTongji UniversityShanghai 200092People’s Republic of China State Key Lab of Physical Chemistry of Solid Surface College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005People’s Republic of China

Metal-air batteries,like Zn-air batteries(ZABs)are usually suffered from low energy conversion efficiency and poor cyclability caused by the sluggish OER and ORR at the air cathode.Herein,a novel bimetallic Co/CoFe nanomaterial supported on nanoflower-like N-doped graphitic carbon(NC)was prepared through a strategy of coordination construction-cation exchange-pyrolysis and used as a highly efficient bifunctional oxygen electrocatalyst.Experimental characterizations and density functional theory calculations reveal the formation of Co/CoFe heterostructure and synergistic effect between metal layer and NC support,leading to improved electric conductivity,accelerated reaction kinetics,and optimized adsorption energy for intermediates of ORR and OER.The Co/CoFe@NC exhibits high bifunctional activities with a remarkably small potential gap of 0.70 V between the half-wave potential(E_(1/2))of ORR and the potential at 10 mA cm^(-2)(E_(j=10))of OER.The aqueous ZAB constructed using this air electrode exhibits a slight voltage loss of only 60 mV after 550-cycle test(360 h,15 days).A sodium polyacrylate(PANa)-based hydrogel electrolyte was synthesized with strong water-retention capability and high ionic conductivity.The quasi-solid-state ZAB by integrating the Co/CoFe@NC air electrode and PANa hydrogel electrolyte demonstrates excellent mechanical stability and cyclability under different bending states.

关键词： Bifunctional electrocatalysts Oxygen electrocatalysis Zn-air battery Co/CoFe heterointerface engineering Density functional theory calculations

A breakthrough in the chemical imaging of single molecule:sub-nm tip-enhanced Raman spectroscopy

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National Science Review 2014年第1期1卷 4-5页

作者： Song-Yuan Ding Zhong-Qun Tian State Key Lab of Physical Chemistry of Solid Surfaces Xiamen University

In 1930,just two years ater his report on‘A New Type of Secondary Radiation’from the scatering of focused beams of sunlight in liquid benzene[1]Sir CV Raman received the Nobel Prize in Physics‘for his work on the scatering of light and for the discovery of the efect named after him’.his great honor was awarded so soon because the scientiic community immediately recognized that the Raman efect could be developed into a powerful ingerprint vibrational spectroscopy

关键词： A breakthrough in the chemical imaging of single molecule SERS nm

Interfacial compatibility issues in rechargeable solid-state lithium metal batteries:a review

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Science China chemistry 2021年第6期64卷 879-898页

作者： Hongchun Wang Jianping Zhu Yu Su Zhengliang Gong Yong Yang College of Energy Xiamen UniversityXiamen 361102China Collaborative Innovation Center of chemistry for Energy Materials State Key Laboratory for Physical Chemistry of Solid SurfaceCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

solid-state lithium metal batteries(SSLBs)contain various kinds of interfaces,among which the solid electrode|solid electrolyte(ED|SE)interface plays a decisive role in the battery's power density and cycling stability.However,it is still lack of comprehensive knowledge and understanding about various interfacial physical/chemical processes so far.Although tremendous efforts have been dedicated to investigate the origin of large interfacial resistance and sluggish charge(electron/ion)transfer process,many scientific and technological challenges still remain to be clarified.In this review,we detach and discuss the critical individual challenge,including charge transfer process,chemical and electrochemical instability,space charge layers,physical contact and mechanical instability.The fundamental concepts,individual effects on the charge transfer and potential solutions are summarized based on material's thermodynamics,electrode kinetics and mechanical effects.It is anticipated that future research should focus on quantitative analysis,modeling analysis and in-situ microstructure characterizations in order to obtain an efficient manipulation about the complex interfacial behaviors in all solid-state Li batteries.

关键词： solid-state lithium metal batteries interfacial compatibility charge transfer kinetics (electro-)chemical stability space charge layer mechanical stability

Anchoring heterometallic cluster on P-doped carbon nitride for efficient photocatalytic nitrogen fixation in water and air ambient

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Chinese Chemical Letters 2024年第4期35卷 176-180页

作者： Chao-Long Chen Rong Chen La-Sheng Long Lan-Sun Zheng Xiang-Jian Kong Collaborative Innovation Center of chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surfaces and Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Light-driven nitrogen fixation to produce ammonia is a green and economical technology of nitrogen reduction but is still quite challenging, especially in an air atmosphere without any sacrificial reagents.Herein, we demonstrate efficient photocatalytic nitrogen fixation using water and air directly by loading lanthanide–transition metal(4f–3d) cluster NdCo_(3) on two-dimensional P-doped graphitic carbon nitrides(PCN) material surface. Benefiting from the increase in the number of nitrogen vacancies(NVs) and highly matched band gap structure and excellent hole trapping ability of clusters, the NdCo_(3)/PCN photocatalyst exhibits efficient nitrogen reduction activity with 371(in air) and 825 μmol h^(-1)g^(-1)(in pure nitrogen)without any sacrificial reagents. The introduction of potassium sulfate inhibits hydrogen production and promotes nitrogen reduction activation. This work suggests that anchoring precisely structured clusters on 2D materials may enhance photocatalytic nitrogen reduction under normal temperature and pressure.

关键词： Photocatalytic Nitrogen fixation 4f-3d Cluster Air atmosphere