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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 ***,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 ***-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 *** integrated AE-CoNDA onto BiVO_(4),photocurrent density of 4.3 mA cm^(−2)is achieved at 1.23 *** 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 *** 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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Polyacrylate modified Cu electrode for selective electrochemical CO_(2) reduction towards multicarbon products

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Science Bulletin 2024年第15期69卷 2395-2404页

作者： Yuchuan Shi Kaini Zhang chung-li dong Ta Thi Thuy Nga Miao Wang Daixing Wei Jialin Wang Yiqing Wang Shaohua Shen International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power EngineeringXi’an Jiaotong UniversityXi’an 710049China Department of Physics Tamkang UniversityNew Taipei City 25137China

Highly selective production of value-added multicarbon(C^(2+))products via electrochemical CO_(2) reduction reaction(eCO_(2)RR)on polycrystalline copper(Cu)remains ***,the facile surface modification using poly(α-ethyl cyanoacrylate)(PECA)is presented to greatly enhance the C^(2+)selectivity for eCO_(2)RR over polycrystalline Cu,with Faradaic efficiency(FE)towards C^(2+)products increased from30.1%for the Cu electrode to 72.6%for the obtained Cu-PECA electrode at-1.1 V *** hydrogen electrode(RHE).Given the well-determined FEs towards C^(2+)products,the partial current densities for C^(2+)production could be estimated to be-145.4 mA cm~(-2)for the Cu-PECA electrode at-0.9 V *** in a homemade flow ***-situ spectral characterizations and theoretical calculations reveal that PECA featured with electron-accepting-C≡N and-COOR groups decorated onto the Cu electrode could inhibit the adsorption of^(*)H intermediates and stabilize the^(*)CO intermediates,given the redistributed interfacial electron density and the raised energy level of d-band center(E_(d))of Cu active sites,thus facilitating the C-C coupling and then the C^(2+)selective *** study is believed to be guidable to the modification of electrocatalysts and electrodes with polymers to steer the surface adsorption behaviors of reaction intermediates to realize practical eCO_(2)RR towards value-added C^(2+)products with high activity and selectivity.

关键词： Electrochemical CO_(2)reduction Polymer modification Electron transfer C_(2+)products

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Chalcogen heteroatoms doped nickel-nitrogen-carbon single-atom catalysts with asymmetric coordination for efficient electrochemical CO_(2)reduction

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Chinese Journal of Catalysis 2024年第9期64卷 54-65页

作者： Jialin Wang Kaini Zhang Ta Thi Thuy Ng Yiqing Wang Yuchuan Shi Daixing Wei chung-li dong Shaohua Shen International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power EngineeringXi'an Jiaotong UniversityXi'an 710049ShaanxiChina Department of Physics Tamkang UniversityNew Taipei City 25137TaiwanChina

The electronic configuration of central metal atoms in single-atom catalysts(SACs)is pivotal in electrochemical CO_(2)reduction reaction(eCO_(2)RR).Herein,chalcogen heteroatoms(e.g.,S,Se,and Te)were incorporated into the symmetric nickel-nitrogen-carbon(Ni-N4-C)configuration to obtain Ni-X-N3-C(X:S,Se,and Te)SACs with asymmetric coordination presented for central Ni *** these obtained Ni-X-N3-C(X:S,Se,and Te)SACs,Ni-Se-N3-C exhibited superior eCO_(2)RR activity,with CO selectivity reaching~98%at-0.70 V versus reversible hydrogen electrode(RHE).The Zn-CO_(2)battery integrated with Ni-Se-N3-C as cathode and Zn foil as anode achieved a peak power density of 1.82 mW cm-2 and maintained remarkable rechargeable stability over 20 ***-situ spectral investigations and theoretical calculations demonstrated that the chalcogen heteroatoms doped into the Ni-N4-C configuration would break coordination symmetry and trigger charge redistribution,and then regulate the intermediate behaviors and thermodynamic reaction pathways for eCO_(2)***,for Ni-Se-N3-C,the introduced Se atoms could significantly raise the d-band center of central Ni atoms and thus remarkably lower the energy barrier for the rate-determining step of*COOH formation,contributing to the promising eCO_(2)RR performance for high selectivity CO production by competing with hydrogen evolution reaction.

关键词： Electrochemical CO_(2)reduction reaction Chalcogen heteroatoms Single-atom catalysts Asymmetric coordination CO production

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Surface sulfurization activating hematite nanorods for efficient photoelectrochemical water splitting

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Science Bulletin 2019年第17期64卷 1262-1271页

作者： lianlian Mao Yu-Cheng Huang Yanming Fu chung-li dong Shaohua Shen International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an 710049 China Department of Physics Tamkang University Tamsui 25137 Taiwan China

Surface treatment is an effective method to improve the photoelectrochemical(PEC) performance of photoelectrodes. Herein, we introduced a novel strategy of surface sulfurization to modify hematite(a-Fe2 O3)nanorods grown in an aqueous solution, which triggered encouraging improvement in PEC *** comparison to the solution-grown pristine a-Fe2 O3 nanorod photoanode that is PEC inefficient and always needs high temperature(>600 °C) activation, the surface sulfurized a-Fe2 O3 nanorods show photocurrent density increased by orders of magnitude, reaching 0.46 mA cmà2 at 1.23 V vs. RHE(reversible hydrogen electrode) under simulated solar illumination. This improvement in PEC performances should be attributed to the synergy of the increased carrier density, the reduced surface charge carrier recombination and the accelerated water oxidation kinetics at the a-Fe2 O3/electrolyte interface, as induced by the incorporation of S ions and the formation of multi-state S species(Fe-Sx-Oy) at the surface of a-Fe2 O3 nanorods. This study paves a new and facile approach to activate a-Fe2 O3 and even other metal oxides as photoelectrodes for improved PEC water splitting performances, by engineering the surface structure to relieve the bottlenecks of charge transfer dynamics and redox reaction kinetics at the electrode/electrolyte interface.

关键词： Photoelectrochemical Water splitting Hematite nanorods Photoanodes Surface sulfurization

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Interlayer ligand engineering of β-Ni(OH)2 for oxygen evolution reaction

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Science China Chemistry 2020年第11期63卷 1684-1693页

作者： Junying He Yuqin Zou Yucheng Huang Chenhui li Yanbo liu ling Zhou chung-li dong Xia Lu Shuangyin Wang State Key Laboratory of Chem/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China Department of Physics Tamkang UniversityNew Taipei City 25137China School of Materials Sun Yat-sen UniversityGuangzhou 510275China

Oxygen evolution reaction(OER)is a bottleneck process for many electrochemical devices due to the sluggish kinetics,for which advanced electrocatalysts should be carefully ***-based materials have been extensively studied to catalyze ***,their performances are still below the expectation and the active sites are often ***,we have successfully modulated the electronic and surface properties of layeredβ-Ni(OH)2 by the interlayer ligand engineering,aiming to design novel efficient electrocatalysts and unveil the catalysis *** one-step solvothermal reaction,alkoxyl substitutedβ-Ni(OH)2 with variable interlayer distances is obtained,and the ethoxyl substituted one(NiEt)shows great potential for efficient *** the assistance of powder X-ray diffraction and crystalline structure computational simulation,the formula of alkoxyl substitutedβ-Ni(OH)2 are *** X-ray absorption spectroscopy studies combined with ex-situ analyses revealed that the critical active species of NiEt is formed via hydroxylation and subsequent de-protonation,with high valent Niδ+(3<δ≤3.66).The corresponding catalytic reaction pathway and mechanism are proposed.

关键词： alkoxyl substitution β-Ni(OH)2 oxygen evolution reaction operando

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Manipulating metal-oxygen local atomic structures in singlejunctional p-Si/WO_(3) photocathodes for efficient solar hydrogen generation

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Nano Research 2021年第7期14卷 2285-2293页

作者： Wu Zhou chung-li dong Yiqing Wang Yu-Cheng Huang lingyun He Han-Wei Chang Shaohua Shen International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power EngineeringXi’an Jiaotong UniversityShaanxi 710049China Department of Physics Tamkang UniversityTamsui 25137TaiwanChina

Self-passivation in aqueous solution and sluggish surface reaction kinetics significantly limit the photoelectrochemical(PEC)performances of silicon-based ***,a WO_(3) thin layer is deposited on the p-Si substrate by pulsed laser deposition(PLD),acting as a photocathode for PEC hydrogen *** to bare p-Si,the single-junctional p-Si/WO_(3) photoelectrodes exhibit excellent and stable PEC performances with significantly increased cathodic photocurrent density and exceptional anodic shift in onset potential for water *** is revealed that the WO_(3) layer could reduce the charge transfer resistance across the electrode/electrolyte interface by eliminating the effect of Fermi level pinning on the surface of *** importantly,by varying the oxygen pressures during PLD,the collaborative modulation of W–O bond covalency and WO6 octahedral structure symmetry contributes to the promoted charge carrier transport and ***,a large band bending at the p-Si/WO_(3) junction,induced by the optimized O vacancy contents in WO_(3),could provide a photovoltage as high as~500 mV to efficiently drive charge transfer to overcome the water reduction ***,by manipulating W–O local atomic structures in the deposited WO_(3) layer,a great improvement in PEC performance could be achieved over the singlejunctional p-Si/WO_(3) photocathodes for solar hydrogen generation.

关键词： silicon local atomic structure water splitting photocathodes hydrogen generation

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In Situ Exfoliation and Pt Deposition of Antimonene for Formic Acid Oxidation via a Predominant Dehydrogenation Pathway

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Research 2020年第1期2020卷 891-901页

作者： Yiqiong Zhang Man Qiao Yucheng Huang Yuqin Zou Zhijuan liu li Tao Yafei li chung-li dong Shuangyin Wang State Key Laboratory of Chemo/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials School of Chemistry and Materials ScienceNanjing Normal UniversityNanjingChina Department of Physics Tamkang UniversityTamsui 25137Taiwan

Direct formic acid fuel cell(DFAFC)has been considered as a promising energy conversion device for stationary and mobile *** platinum(Pt)electrocatalysts for formic acid oxidation reaction(FAOR)are critical for ***,the oxidation of formic acid on Pt catalysts often occurs via a dual pathway mechanism,which hinders the catalytic activity owing to the CO ***,we directly exfoliate bulk antimony to 2D antimonene(Sb)and in situ load Pt nanoparticles onto antimonene sheets with the assistance of *** to the Bader charge analysis,the charge transfer from antimonene to Pt occurs,confirming the electronic interaction between Pt and ***,antimonene,as a cocatalyst,alters the oxidation pathway for FAOR over Pt catalyst and makes FAOR follow the more efficient dehydrogenation *** density functional theory(DFT)calculation demonstrates that antimonene can activate Pt to be a lower oxidative state and facilitate the oxidation of HCOOH into CO_(2) via a direct pathway,resulting in a weakened intermediate binding strength and better CO tolerance for *** specific activity of FAOR on Pt/Sb is 4.5 times,and the mass activity is 2.6 times higher than the conventional Pt/C.

关键词： catalyst charge oxidative

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Regulation on polymerization degree and surface feature in graphitic carbon nitride towards efficient photocatalytic H2 evolution under visible-light irradiation

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Journal of Materials Science & Technology 2022年第3期98卷 160-168页

作者： Cheng Cheng chung-li dong Jinwen Shi liuhao Mao Yu-Cheng Huang Xing Kang Shichao Zong Shaohua Shen International Research Center for Renewable Energy(IRCRE) State Key Laboratory of Multiphase Flow in Power Engineering(MFPE)Xi'an Jiaotong University(XJTU)28 West Xianning RoadXi’an 710049China Department of Physics Tamkang University151 Yingzhuan RoadTamsui 25137TaiwanChina

A kind of graphitic carbon nitride(TSC-550) with high polymerization degree and improved surface property was prepared by a new precursor of thiosemicarbazide. The sulfur motif and high nitrogen content in thiosemicarbazide promoted the polymerization of thiosemicarbazide to form graphitic carbon nitride framework with high degree of polymerization, which significantly influenced the electronic structure and surface chemical properties. TSC-550 possessed a narrow bandgap of 2.19 eV that facilitated the utilization of visible light, and possessed a less positive charge, acidic surface that resulted in enhanced hydrogen adsorption ability in water solution, which promoted the H;evolution kinetics. In addition, the extended π-conjugated electronic system promoted the separation and migration of photogenerated charge carries in plane of TSC-550 framework, as well as the increasing interlayer C–N interactions in TSC-550 created conductive paths across the layers to tunnel interlayers for rapid electron transportation. As a result, TSC-550 nanosheets showed excellent photocatalytic H;production activity,the AQY achieved 36.4% at 425 nm.

关键词： Degree of polymerization Graphitic carbon nitride Photocatalysis Solar energy Hydrogen

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Promoting surface reconstruction of NiFe layered double hydroxides via intercalating[Cr(C_(2)O_(4))_(3)]^(3-)for enhanced oxygen evolution

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Journal of Energy Chemistry 2022年第11期31卷 140-148,I0005页

作者： Yujie Wu Minglei Song Yu-Cheng Huang chung-li dong Yingying li Yuxuan Lu Bo Zhou dongdong Wang Jianfeng Jia Shuangyin Wang Yanyong Wang State Key Laboratory of Chemo/Bio-Sensing and Chemometrics College of Chemistry and Chemical Engineeringthe National Supercomputing Center in ChangshaHunan UniversityChangsha 410082HunanChina Department of Physics Tamkang UniversityNew Taipei City 25137TaiwanChina Key Laboratory of Magnetic Molecules and Magnetic Information Materials(Ministry of Education) School of Chemistry and Material ScienceShanxi Normal UniversityTaiyuan 030031ShanxiChina

Rationally manipulating surface reconstruction of catalysts for water oxidation,inducing formation and dynamic accumulation of catalytically active centers still face numerous ***,the introduction of[Cr(C_(2)O_(4))_(3)]^(3-)into NiFe LDHs by intercalation engineering to promote surface reconstruction achieves an advanced oxygen evolution reaction(OER)*** view of the weak electronegativity of Cr^(3+) in[Cr(C_(2)O_(4))_(3)]^(3-),the intercalation of[Cr(C_(2)O_(4))_(3)]^(3-)is expected to result in an electron-rich structure of Fe sites in NiFe LDHs,and higher valence state of Ni can be formed with the charge transfer between Fe and *** optimized electronic structure of NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs with more active Ni^(3+) species and the expedited dynamic generation of Ni^(3+) (Fe)OOH phase during the OER process contributed to its excellent catalytic property,revealed by in situ X-ray absorption spectroscopy,Raman spectroscopy,and quasi-in situ X-ray photoelectron *** the modulated electronic structure of metal sites,NiFe-[Cr(C_(2)O_(4))_(3)]^(3-)-LDHs exhibited promoted OER property with a lower overpotential of 236 mV at the current density of 10 mA cm^(-2).This work illustrates the intercalation of conjugated anion to dynamically construct desired Ni^(3+) sites with the optimal electronic environment for improved OER electrocatalysis.

关键词： NiFe layered double hydroxides [Cr(C_(2)O_(4))_(3)]^(3-)intercalation Dynamic restructuring Operando spectroscopies Oxygen evolution reaction

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Hierarchically nanostructured Ni O-Co3O4 with rich interface defects for the electro-oxidation of 5-hydroxymethylfurfural

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Science China Chemistry 2020年第7期63卷 980-986页

作者： Yuxuan Lu chung-li dong Yu-Cheng Huang Yuqin Zou Yanbo liu Yingying li Nana Zhang Wei Chen ling Zhou Hongzhen lin Shuangyin Wang State Key Laboratory of Chem/Bio-Sensing and Chemometrics Provincial Hunan Key Laboratory for Graphene Materials and DevicesCollege of Chemistry and Chemical Engineeringthe National Supercomputer Centers in ChangshaHunan UniversityChangsha 410082 Department of Physics Tamkang UniversityTaipei 25137 i-LAB Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123

Ni-based electrocatalysts with strong redox abilities are active for the electrochemical oxidation of 5-hydroxymethylfurfural(HMF). Interface engineering is an efficient way to modulate the electronic structure, tune the intermediate adsorption, and expose more active sites. Herein, we increased the concentration of interfacial sites with rich defects in a 3D hierarchical nanostructured NiO-Co3O4 electrocatalyst and investigated its catalytic performance for HMF electro-oxidation. The interface effect created abundant cation vacancies, modulated the electronic properties of Co and Ni atoms, and raised the oxidation state of Ni species. The NiO-Co3O4 catalysts show superb HMF oxidation activities with a low onset potential of 1.28 ***, in-situ surface-selective vibrational spectroscopy of sum-frequency generation was performed to study the reaction pathway during the oxidation process on the electrocatalysts. The current study offers an efficient way to create cation vacancies and proves the decisive role of cation vacancies in catalyzing the HMF electro-oxidation.

关键词： interface effect cation vacancies in-situ vibrational spectroscopy electrochemical biomass conversion 3D hierarchical nanostructure

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