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electronic structure regulation and built-in electric field synergistically strengthen photocatalytic nitrogen fixation performance on Ti-BiOBr/TiO_(2)heterostructure

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Rare Metals 2024年第3期43卷 1125-1138页

作者： Ru-Qi Li Yu-Jie Bian Chun-Ming Yang Li Guo Tao-Xia Ma Chuan-Tao Wang Feng Fu Dan-Jun Wang College of Chemistry and Chemical Engineering Yan’an UniversityYan’an Key Laboratory of Green Catalysis and Quality Improvement and Utilization of Low Rank CoalYan’an716000China

At present,industrial synthetic ammonia was still obtained through the Hubble-Bosch process,with large energy *** is a research hotspot to realize green synthetic ammonia by using solar *** difficulty of photocatalytic ammonia synthesis was that the photo-excited electrons have not enough energy to active N≡*** this study,Ti was doped into BiOBr by one-step hydrothermal method,which was oxidized into TiO_(2)when the doping amount reaches the maximum,in situ forming Ti_(0.31)B_(0.69)OB/TiO_(2)*** from the synergistic effect of Ti doping and S-scheme heterojunction,the synthetic ammonia efficiency of Ti_(0.31)B_(0.69)OB/TiO_(2)-11.96 reached 1.643 mmol·g_(cat)^(-1)at mild conditions and without hole scavenger for up to 7 h,the efficiency of synthetic ammonia is 115 times,10.5 times and 3.3 times of that of BiOBr,Ti_(0.31)B_(0.69)OB and TiO_(2),***,DFT calculation confirms that Ti doping accurately refine the electronic structure of BiOBr,facilitate nitrogen adsorption activation and reduce hydrogenation reaction energy barrier,thus accelerating the reaction kinetics of photocatalytic nitrogen reduction(NRR),Meanwhile,constructing S-scheme heterojunction boosts the separation and transfer of photogenerated electron-hole pairs,improving the reduction ability of electrons in the conduction band of TiO_(2)and the oxidation ability of holes in the valence band of Ti_(0.31)B_(0.69)OB.

关键词： S-scheme heterostructure electronic structure regulation Built-in electric field Synergistical stren4gthening Photocatalytic nitrogen fixation

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High-performance Bi_(2)S_(3)/ZnO photoanode enabled by interfacial engineering with oxyanion for efficient photoelectrochemical water oxidation

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Nano Research 2024年第7期17卷 5996-6005页

作者： Ying-Chu Chen Hsiang-Yu Jui Yichen Feng Yun-Hsiang Lu Yu-Kuei Hsu Department of Chemical Engineering&Biotechnology "National Taipei University of Technology"No.1Sec.3Zhong-Xiao E.Rd.Da'an Dist.Taipei City 10608TaiwanChina Department of Opto-electronic Engineering "National Dong Hwa University"No.1Sec.2Da Hsueh RoadShoufengHualien 97401TaiwanChina China-UK Low Carbon College Shanghai Jiao Tong UniversityNo.3Yinlian RoadLingangShanghai 201306China

In the present contribution,we demonstrate that the sluggish kinetics of oxygen evolution reaction(OER)over the bismuth sulfide(Bi_(2)S_(3))photoanode,which severely restricts its photoelectrochemical activity,is markedly accelerated by employing a sulfatecontaining ***-principle calculation points to the spontaneous adsorption of sulfate(SO_(4)^(2−))on Bi_(2)S_(3)and its capacity of stabilizing the OER intermediates through hydrogen bonding,which is further reinforced by increasing the local density of states near the Fermi level of Bi_(2)S_(3).Meanwhile,the electron transfer is also promoted to synergistically render the ratedetermining step(from O*to OOH*)of OER over Bi_(2)S_(3)kinetically *** but not least,benefitting from such enhanced OER activity and efficient charge separation resulted from depositing Bi_(2)S_(3)on the zinc oxide nanorods(ZnO NRs),forming a core–shell heterojunction,its photocurrent density achieves 8.61 mA·cm^(−2)at 1.23 VRHE,far surpassing those reported for additional Bi_(2)S_(3)-based and several state-of-the-art photoanodes in the literature and further exceeding their theoretical *** great promise of the Bi_(2)S_(3)/ZnO NRs is in view of such outperformance,the superior Faradaic yield of oxygen of more than~80%and the outstanding half-cell applied bias photon-to-current efficiency of~1%well corroborated.

关键词： photoelectrochemical water oxidation oxyanion adsorption electronic structure regulation oxygen evolution reaction(OER)intermediates stabilization Bi_(2)S_(3)

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Single-atom sites regulation by the second-shell doping for efficient electrochemical CO_(2)reduction

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Chinese Chemical Letters 2024年第9期35卷 360-363页

作者： Qian-Qian Tang Li-Fang Feng Zhi-Peng Li Shi-Hao Wu Long-Shuai Zhang Qing Sun Mei-Feng Wu Jian-Ping Zou Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle Nanchang Hangkong UniversityNanchang 330063China National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization Nanchang Hangkong UniversityNanchang 330063China

Nitrogen-doped carbon loaded single-atom catalysts(SACs)are promising candidates for electrocatalytic conversion of CO_(2)into high-valuable chemicals,and the modification of catalysts by heteroatom-doping strategy is an effective approach to enhance the CO_(2)reduction ***,the large difference exists in atomic radius between nitrogen atoms and the doped heteroatoms may lead to the poor stability of active *** this study,we have synthesized a Ni single atom catalyst with S doping at the secondshell on the ultrathin carbon nanosheets support(Ni-N_(4)-SC)by solid-phase *** S atom in the second-shell contributes to the higher efficiency of CO_(2)conversion at lower potentials while the Ni-N_(4)-SC can be more *** experimental results and theoretical calculations indicate that the S atom in second-shell breaks the uniform charge distribution and reduces the free energy of hydrogenation,which can increase the adsorption of CO_(2),accelerate charge transfer,and reduce the reaction energy *** work reveals the close relationship between the second-shell and the electrocatalytic activity of single atom sites,which also provides a new perspective to design efficient single atom catalysts.

关键词： Single-atom catalyst Heteroatom-doping Second shell CO_(2)electroreduction electronic structure regulation

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Regulating electronic structure of CoN_(4)with axial Co-S for promoting oxygen reduction and Zn-air battery performance

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Nano Research 2023年第4期16卷 4211-4218页

作者： Chang Chen Zhiqiang Chen Junxi Zhong Xin Song Dongfang Chen Shoujie Liu Weng-Chon Cheong Jiazhan Li Xin Tan Chang He Jiaqi Zhang Di Liu Qiuhua Yuan Chen Chen Qing Peng Yadong Li Department of Chemistry Tsinghua UniversityBeijing 100084China Beijing Key Laboratory of Research and Application for Aerospace Green Propellants Beijing Institute of Aerospace Testing TechnologyBeijing 100048China College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China State Key Laboratory of Automtive Safety and Energy Tsinghua UniversityBeijing 100084China Chemistry and Chemical Engineering Guangdong Laboratory Shantou 515031China Department of Physics and Chemistry Faculty of Science and TechnologyUniversity of MacaoMacao 999078China

Regulating the coordination environment of transition-metal based materials in the axial direction with heteroatoms has shown great potential in boosting the oxygen reduction reaction(ORR).The coordination configuration and the regulation method are pivotal and ***,we report a combined strategy of matrix-activization and controlled-induction to modify the CoN_(4)site by axial coordination of Co-S(Co1N_(4)-S_(1)),which was validated by the aberration-corrected electron microscopy and X-ray absorption fine structure *** optimal Co1N_(4)-S_(1)exhibits an excellent alkaline ORR activity,according to the half-wave potential(0.897 V *** hydrogen electrode(RHE)),Tafel slope(24.67 mV/dec),and kinetic current ***,the Co1N_(4)-S_(1)based Zn-air battery displays a high power density of 187.55 mW/cm^(2)and an outstanding charge-discharge cycling stability for 160 h,demonstrating the promising application *** calculations indicate that the better regulation of CoN_(4)on electronic structure and thus the highly efficient ORR performance can be achieved by axial Co-S.

关键词： electronic structure regulation axial Co-S coordination single-atom Co oxygen reduction Zn-air battery

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Modulate the electronic structure of Cu_(7)S_(4)nanosheet on TiO_(2)for enhanced photocatalytic hydrogen evolution

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Nano Research 2023年第4期16卷 4488-4493页

作者： Wenqiang Liu Huiping Peng Leigang Li Mingmin Wang Hongbo Geng Xiaoqing Huang State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China School of Materials Engineering Changshu Institute of TechnologyChangshu 215500China

TiO_(2)is a promising photocatalyst due to its high thermodynamic stability and ***,its applications have been still limited because of the high recombination rate of electron-hole ***,we show that by combining heterojunction construction and electronic structure regulation,the electron-hole pairs in TiO_(2)can be effectively separated for enhanced photocatalytic hydrogen *** optimized Cu_(7)S_(4)nanosheet decorated TiO_(2)achieves much enhanced H_(2)evolution rate(11.5 mmol·g−1·h−1),which is 13.8 and 4.2 times of that of TiO_(2)and Cu_(7)S_(4)/TiO_(2),*** results of photoluminescence spectroscopy,transient photocurrent spectra,ultraviolet-visible diffuse reflectance spectra,and electrochemical impedance spectroscopy collectively demonstrate that the enhanced photocatalytic performance of Air-Cu_(7)S_(4)/TiO_(2)is attributed to the effective separation of charge carriers and widened photoresponse *** electron paramagnetic resonance and X-ray photoelectron spectroscopy results indicate that the increase of Cu2+in the Cu_(7)S_(4)nanosheet after calcination can promote the charge *** work provides an effective method to improve the electron migration rate and charge separation of TiO_(2),which holds great significance for being extended to other material systems and beyond.

关键词： Cu_(7)S_(4)nanosheet Cu^(2+) electronic structure regulation heterojunction photocactalytic hydrogen evolution

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electronic modulation of two-dimensional bismuth-based nanosheets for electrocatalytic CO_(2) reduction to formate: A review

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Materials Reports(Energy) 2023年第1期3卷 51-64,I0002页

作者： Guan Wang Fangyuan Wang Peilin Deng Jing Li Chongtai Wang Yingjie Hua Yijun Shen Xinlong Tian State Key Laboratory of Marine Resource Utilization in South China Sea Hainan Provincial Key Lab of Fine ChemistrySchool of Chemical Engineering and TechnologyHainan UniversityHaikou570228China Key Laboratory of Electrochemical Energy Storage and Energy Conversion of Hainan Province School of Chemistry and Chemical EngineeringHainan Normal UniversityHaikou571158China

Electrocatalytic CO_(2) reduction reaction(eCO_(2) RR)has significant relevance to settle the global energy crisis and abnormal climate problem via mitigating the excess emission of waste CO_(2) and producing high-value-added ***,eCO_(2) RR to formic acid or formate is one of the most technologically and economically viable approaches to realize high-efficiency CO_(2) utilization,and the development of efficient electrocatalysts is very urgent to achieve efficient and stable catalytic *** this review,the recent advances for two-dimensional bismuth-based nanosheets(2D Bi-based NSs)electrocatalysts are concluded from both theoretical and experimental ***,the preparation strategies of 2D Bi-based NSs in aspects to precisely control the thickness and uniformity are *** addition,the electronic regulation strategies of 2D Bi-based NSs are highlighted to gain insight into the effects of the structure-property relationship on facilitating CO_(2) activation,improving product selectivity,and optimizing carrier transport ***,the considerable challenges and opportunities of 2D Bi-based NSs are discussed to lighten new directions for future research of eCO_(2) RR.

关键词： CO_(2) electroreduction Two-dimensional structure Bismuth-based catalysts Preparation strategy electronic structure regulation Formate

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