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1T′‐MoTe_(2) monolayer:A promising two‐dimensional catalyst for the electrochemical production of hydrogen peroxide
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作者 Xiaoxu Sun Xiaorong Zhu +1 位作者 Yu Wang Yafei Li 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第6期1520-1526,共7页
The direct synthesis of hydrogen peroxide(H_(2)O_(2))via a two‐electron oxygen reduction reaction(2e‐ORR)in acidic media has emerged as a green process for the production of this valuable chemical.However,such an ap... The direct synthesis of hydrogen peroxide(H_(2)O_(2))via a two‐electron oxygen reduction reaction(2e‐ORR)in acidic media has emerged as a green process for the production of this valuable chemical.However,such an approach employs expensive noble‐metal‐based electrocatalysts,which severely undermines its feasibility when implemented on an industrial scale.Herein,based on density functional theory computations and microkinetic modeling,we demonstrate that a novel two‐dimensional(2D)material,namely a 1T′‐MoTe_(2)monolayer,can serve as an efficient non‐precious electrocatalyst to facilitate the 2e‐ORR.The 1T′‐MoTe_(2)monolayer is a stable 2D crystal that can be easily produced through exfoliation techniques.The surface‐exposed Te sites of the 1T′‐MoTe_(2)monolayer exhibit a favorable OOH*binding energy of 4.24 eV,resulting in a rather high basal plane activity toward the 2e‐ORR.Importantly,kinetic computations indicate that the 1T'‐MoTe_(2)monolayer preferentially promotes the formation of H_(2)O_(2)over the competing four‐electron ORR step.These desirable characteristics render 1T′‐MoTe_(2)a promising candidate for catalyzing the electrochemical reduction of O_(2)to H_(2)O_(2). 展开更多
关键词 1T′‐MoTe_(2) Two‐dimensional catalyst electrochemical H_(2)O_(2) production Density functional theory computations Microkinetic modeling
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Synergistic effect of size-dependent PtZn nanoparticles and zinc single-atom sites for electrochemical ozone production in neutral media 被引量:1
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作者 Bowen Yuan Zihao Yao +7 位作者 Chenlong Qiu Haiyang Zheng Yilong Yan Qiaoqiao Zhang Xiang Sun Yu Gu Xing Zhong Jianguo Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2020年第12期312-322,共11页
Electrochemical ozone production(EOP) via water electrolysis represents an attractive method for the generation of high-purity O3. Herein, the X-PtZn/Zn-N-C electrocatalysts show a strong structural sensitive behavior... Electrochemical ozone production(EOP) via water electrolysis represents an attractive method for the generation of high-purity O3. Herein, the X-PtZn/Zn-N-C electrocatalysts show a strong structural sensitive behavior depends on the size of the PtZn nanoparticles and their EOP activity exhibits a volcano-type dependence for the O3 performance in neutral media. The 7.7-PtZn/Zn-N-C exhibits EOP current efficiency of 4.2%, and shows the prominent performance in the production of gaseous O3 with a value of 1647 ppb at 30 min, which is almost 4-fold compared to 2.2-Pt Zn/Zn-N-C. Based on the experiments and theoretical calculations, the performance of the EOP process was determined by the nanoparticle size-effect and the synergistic effect between the PtZn nanoparticles and atomically dispersed Zn-N-C. Furthermore, the fivemembered cyclic structure of O3 can be stabilized between the PtZn nanoparticle and the Zn-N-C support,indicating that O3 is produced at the interface. 展开更多
关键词 electrochemical ozone production PtZn Single-atom catalysts Size effect Synergistic effect
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Phosphorous and selenium tuning Co-based non-precious catalysts for electrosynthesis of H_(2)O_(2)in acidic media 被引量:1
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作者 Jingxin Xie Lijie Zhong +6 位作者 Xin Yang Dequan He Kanglong Lin Xiaoxia Chen Huan Wang Shiyu Gan Li Niu 《Chinese Chemical Letters》 SCIE CAS CSCD 2024年第1期475-481,共7页
Electrosynthesis of hydrogen peroxide(H2O2)is an on-site method that enables independent distribution applications in many fields due to its small-scale and sustainable features.The crucial point remains developing hi... Electrosynthesis of hydrogen peroxide(H2O2)is an on-site method that enables independent distribution applications in many fields due to its small-scale and sustainable features.The crucial point remains developing highly active,selective and cost-effective electrocatalysts.The electrosynthesis of H2O2 in acidic media is more practical owing to its stability and no need for further purification.We herein report a phosphorus and selenium tuning Co-based non-precious catalyst(CoPSe)toward two-electron oxygen reduction reaction(2e–ORR)to produce H2O2 in acidic media.The starting point of using both P and Se is finding a balance between strong ORR activity of CoSe and weak activity of CoP.The results demonstrated that the CoPSe catalyst exhibited the optimized 2e–ORR activity compared with CoP and CoSe.It disclosed an onset potential of 0.68 V and the H2O2 selectivity 76%-85%in a wide potential range(0–0.5 V).Notably,the CoPSe catalyst overcomes a significant challenge of a narrow-range selectivity for transitionmetal based 2e–ORR catalysts.Finally,combining with electro-Fenton reaction,an on-site system was constructed for efficient degradation of organic pollutants.This work provides a promising non-precious Co-based electrocatalyst for the electrosynthesis of H2O2 in acidic media. 展开更多
关键词 Oxygen reduction reaction electrochemical H2O2 production ELECTROCATALYSIS Non-precious electrocatalyst Acidic media
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Heterophase junction engineering-induced Co spin-state modulation of CoSe_(2) for large-current hydrogen evolution reaction
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作者 Bao-Chai Xu Ya-Ping Miao +9 位作者 Min-Qin Mao Dong-Lian Li Song Xie Wei-Hong Jin Shu Xiao Jing Wen Zaenab Abd-Allah Zhi-Tian Liu Xiang Peng Paul K.Chu 《Rare Metals》 SCIE EI CAS CSCD 2024年第6期2660-2670,共11页
Efficient electrocatalysts are vital to large-current hydrogen production in commercial water splitting for green energy generation.Herein,a novel heterophase engineering strategy is described to produce polymorphic C... Efficient electrocatalysts are vital to large-current hydrogen production in commercial water splitting for green energy generation.Herein,a novel heterophase engineering strategy is described to produce polymorphic CoSe_(2)electrocatalysts.The composition of the electrocatalysts consisting of both cubic CoSe_(2)(c-CoSe_(2))and orthorhombic CoSe_(2)(o-CoSe_(2))phases can be controlled precisely.Our results demonstrate that junction-induced spin-state modulation of Co atoms enhances the adsorption of intermediates and accelerates charge transfer resulting in superior large-current hydrogen evolution reaction(HER)properties.Specifically,the CoSe_(2)based heterophase catalyst with the optimal c-CoSe_(2)content requires an overpotential of merely 240 mV to achieve 1,000 mA·cm^(-2)as well as a Tafel slope of 50.4 mV·dec^(-1).Furthermore,the electrocatalyst can maintain a large current density of 1,500 mA·cm^(-2)for over 320 h without decay.The results reveal the advantages and potential of heterophase junction engineering pertaining to design and fabrication of low-cost transition metal catalysts for large-current water splitting. 展开更多
关键词 Heterophase junction SPIN-STATE Hydrogen evolution reaction Large current electrochemical hydrogen production Water splitting
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Fullerene-derived boron-doped defective nanocarbon for highly selective H_(2)O_(2) electrosynthesis
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作者 Wangqiang Shen Chang Zhang +7 位作者 Muneerah Alomar Zhiling Du Zepeng Yang Junjie Wang Guangqing Xu Jian Zhang Jun Lv Xing Lu 《Nano Research》 SCIE EI CSCD 2024年第3期1217-1224,共8页
Electrochemical production of hydrogen peroxide(H_(2)O_(2))via the two-electron(2e-)pathway of oxygen reduction reaction(ORR)supplies an auspicious alternative to the current industrial anthraquinone process.Nonethele... Electrochemical production of hydrogen peroxide(H_(2)O_(2))via the two-electron(2e-)pathway of oxygen reduction reaction(ORR)supplies an auspicious alternative to the current industrial anthraquinone process.Nonetheless,it still lacks efficient electrocatalysts to achieve high ORR activity together with 2e-selectivity simultaneously.Herein,a boron-doped defective nanocarbon(B-DC)electrocatalyst is synthesized by using fullerene frameworks as the precursor and boric oxide as the boron source.The obtained B-DC materials have a hierarchical porous structure,befitting boron dopants,and abundant topological pentagon defects,exhibiting a high ORR onset potential of 0.78 V and a dominated 2e-selectivity(over 95%).Remarkably,when B-DC electrocatalyst is employed in a real device,it achieves a high H_(2)O_(2) yield rate(247 mg·L^(-1)·h^(-1)),quantitative Faraday efficiency(~100%),and ultrafast organic pollutant degradation rate.The theoretical calculation reveals that the synergistic effect of topological pentagon defects and the incorporation of boron dopants promote the activation of the O_(2) molecule and facilitates the desorption of oxygen intermediate.This finding will be very helpful for the comprehension of the synergistic effect of topological defects and heteroatom dopants for boosting the electrocatalytic performance of nanocarbon toward H_(2)O_(2) production. 展开更多
关键词 FULLERENE electrochemical hydrogen peroxide production oxygen reduction reaction carbon nanomaterials
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Water flooding behavior in flow cells for ammonia production via electrocatalytic nitrogen reduction 被引量:1
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作者 Zhefei Pan Farhan Khalid +4 位作者 Abdullah Tahir Oladapo Christopher Esan Jie Zhu Rong Chen Liang An 《Fundamental Research》 CAS 2022年第5期757-763,共7页
The green production of ammonia,in an electrochemical flow cell under ambient conditions,is a promising way to replace the energy-intensive Haber-Bosch process.In the operation of this flow cell with an alkaline elect... The green production of ammonia,in an electrochemical flow cell under ambient conditions,is a promising way to replace the energy-intensive Haber-Bosch process.In the operation of this flow cell with an alkaline electrolyte,water is produced at the anode but also required as an essential reactant at the cathode for nitrogen reduction.Hence,water from the anode is expected to diffuse through the membrane to the cathode to compensate for the water needed for nitrogen reduction.Excessive water permeation,however,tends to increase the possibility of water flooding,which would not only create a large barrier for nitrogen delivery and availability,but also lead to severe hydrogen evolution as side reaction,and thus significantly lower the ammonia production rate and Faradaic efficiency.In this work,the water flooding phenomenon in flow cells for ammonia production via electrocatalytic nitrogen reduction is verified via the visualization approach and the electrochemical cell performance.In addition,the effects of the nitrogen flow rate,applied current density,and membrane thickness on the water crossover flux and ammonia production rate are comprehensively studied.The underlying mechanism of water transport through the membrane,including diffusion and electro-osmotic drag,is precisely examined and specified to provide more insight on water flooding behavior in the flow cell. 展开更多
关键词 Nitrogen reduction electrochemical ammonia production Flow cells Water flooding Water transport Operation conditions
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The Structural and Chemical Reactivity of Lattice Oxygens on β-PbO_(2 ) EOP Electrocatalysts 被引量:2
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作者 Wenwen Li Ge Feng +5 位作者 Jia Liu Xing Zhong Zihao Yao Shengwei Deng Shibin Wang Jianguo Wang 《Chinese Journal of Structural Chemistry》 SCIE CAS CSCD 2022年第12期51-59,共9页
The oxygen evolution reaction(OER)and electrochemical ozone production(EOP)attracted considerable attention due to their wide applications in electrocatalysis,but the detailed reaction mechanism of product formation a... The oxygen evolution reaction(OER)and electrochemical ozone production(EOP)attracted considerable attention due to their wide applications in electrocatalysis,but the detailed reaction mechanism of product formation as well as the voltage effect on O_(2)/O_(3)formation still remains unclear.In this work,density functional theory calculations were used to systematically investigate the possible reaction mechanisms of OER and EOP on the PbO_(2)(110)surface,with the possible reaction network involving surface lattice oxygen atoms(LOM)proposed.The results show that the LOM-2 reaction pathway involving two surface lattice oxygen atoms(Olatt)and one oxygen atom from H_(2)O was the most thermodynamically reactive.Different potential determining step(PDS)was obtained depending on the multiple reaction pathway,and the results show that the facile diffusion of Olattwould proceed the LOM pathway and promote the formation of surface oxygen vacancies(O_(vac1)/O_(vac2)).Furthermore,O_(vac1)/O_(vac2)formation on the surface would trigger further reactions of H_(2)O adsorption and splitting,which refilled the oxygen vacancy and ensured the considerable stability of the PbO_(2)(110)surface.Multiple H_(2)O dissociation pathways were proposed on PbO_(2)(110)with oxygen vacancy sites:the acid-base interaction mechanism and the vacancy fulfilling mechanism. 展开更多
关键词 oxygen vacancy effect electrochemical ozone production lattice oxygen mechanism density functional theory
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Corrosion Evolution of Low Alloy Steel in Deaerated Bicarbonate Solutions 被引量:2
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作者 Yunfei Lu Junhua Dong Wei Ke 《Journal of Materials Science & Technology》 SCIE EI CAS CSCD 2015年第10期1047-1058,共12页
Corrosion evolution during immersion tests (up to 43 days) of NiCu steel in deaerated 0.1 mol/L bicarbonate solutions was investigated by electrochemical measurements, scanning electron microscopy (SEM) and X-ray ... Corrosion evolution during immersion tests (up to 43 days) of NiCu steel in deaerated 0.1 mol/L bicarbonate solutions was investigated by electrochemical measurements, scanning electron microscopy (SEM) and X-ray diffraction (XRD). Results show that NiCu steel transformed from the anodic dissolution in the early stage of immersion to a metastable passive state in the final stage as the open-circuit potential value shifted positively, which was aroused by the precipitation of corrosion products. This process was mainly promoted by the trace amount of oxygen. Simultaneously, dominant cathodic reaction transformed from the hydrogen evolution in early stage to reduction processes of corrosion products in later stages. Possible corrosion processes were discussed with the assistance of a corresponding Pourbaix diagram. 展开更多
关键词 Low alloy steelCorrosion behaviour Potential Corrosion product film Potentiodynamic polarization electrochemical impedance spectroscopy(EIS)
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