Enhancing catalytic activity through modulating the interaction between N-doped carbon and metal phosphides clusters is an effective approach.Herein,the electronic structure modulation of CoP_(2) supported N-modified ...Enhancing catalytic activity through modulating the interaction between N-doped carbon and metal phosphides clusters is an effective approach.Herein,the electronic structure modulation of CoP_(2) supported N-modified carbon(CoP_(2)/NC)has been designed and prepared as efficient electrocatalysts for oxygen reduction reaction(ORR),oxygen evolution reaction(OER),and hydrogen evolution reaction(HER).Notably,CoP_(2)/NC-1 catalyst exhibits impressive performance in alkaline media,with an ORR half-wave potential of 0.84 V,as well as OER and HER overpotentials of 290 and 129 mV(at 10 mA·cm^(−2)),respectively.In addition,CoP_(2)/NC-1 produces a power density as high as 172.9 mW·cm^(−2),and excellent reversibility of 100 h at 20 mA·cm^(−2) in home-made Zn-air batteries.The experimental results demonstrate that the synergistic interactions between N modified carbon substrate and CoP_(2) material significantly enhance the kinetics of ORR,OER,and HER.Density functional theory(DFT)calculations reveal the strong electrons redistribution of CoP_(2) induced by high-density N atoms at the interface,thus optimizing the key intermediates and significantly lower the energy barrier of reactions.These electronic adjustments of CoP_(2) greatly enhance its kinetics of ORR/OER/HER,leading to faster reactions.This study provides profound insights into the specific modification of CoP_(2) by N-doped carbon,enabling the construction of efficient catalysts.展开更多
The development of e cient earth-abundant electrocatalysts for oxygen reduction, oxygen evolution, and hydrogen evolution reactions(ORR, OER, and HER) is important for future energy conversion and energy storage devic...The development of e cient earth-abundant electrocatalysts for oxygen reduction, oxygen evolution, and hydrogen evolution reactions(ORR, OER, and HER) is important for future energy conversion and energy storage devices, for which both rechargeable Zn–air batteries and water splitting have raised great expectations. Herein, we report a single-phase bimetallic nickel cobalt sulfide((Ni,Co)S_2) as an e cient electrocatalyst for both OER and ORR. Owing to the synergistic combination of Ni and Co, the(Ni,Co)S_2 exhibits superior electrocatalytic performance for ORR, OER, and HER in an alkaline electrolyte, and the first principle calculation results indicate that the reaction of an adsorbed O atom with a H_2O molecule to form a *OOH is the potential limiting step in the OER. Importantly, it could be utilized as an advanced air electrode material in Zn–air batteries, which shows an enhanced charge–discharge performance(charging voltage of 1.71 V and discharge voltage of 1.26 V at 2 mA cm^(-2)), large specific capacity(842 mAh g_(Zn)^(-1) at 5 mA cm^(-2)), and excellent cycling stability(480 h). Interestingly, the(Ni,Co)S_2-based Zn–air battery can e ciently power an electrochemical water-splitting unit with(Ni,Co)S_2 serving as both the electrodes. This reveals that the prepared(Ni,Co)S_2 has promising applications in future energy conversion and energy storage devices.展开更多
In order to investigate whether an air–water plasma jet is beneficial to improve the efficiency of inactivation, a series of experiments were done using a ring-needle plasma jet. The water content in the working gas...In order to investigate whether an air–water plasma jet is beneficial to improve the efficiency of inactivation, a series of experiments were done using a ring-needle plasma jet. The water content in the working gas（air） was accurately measured based on the Karl Fischer method. The effects of water on the production of OH（A;Σ;–X;Π;） and O（3p;P–3s;S） were also studied by optical emission spectroscopy. The results show that the water content is in the range of 2.53–9.58 mg l;, depending on the gas/water mixture ratio. The production of OH（A;Σ;–X;Π;） rises with the increase of water content, whereas the O（3p;P–3s;S） shows a declining tendency with higher water content. The sterilization experiments indicate that this air–water plasma jet inactivates the P. digitatum spores very effectively and its efficiency rises with the increase of the water content. It is possible that OH（A;Σ;–X;Π;） is a more effective species in inactivation than O（3p;P–3s;S） and the water content benefit the spore germination inhibition through rising the OH（A;Σ;–X;Π;） production. The maximum of the inactivation efficacy is up to 93% when the applied voltage is -6.75 kV and the water content is 9.58 mg l;.展开更多
基金supported by the National Natural Science Foundation of China(Nos.51872209,52171145,21972106,22105146)Zhejiang Province Natural Science Foundation project key project(No.LZ20B030001)Zhejiang Provincial Special Support Program for High-level Talents(No.2019R52042).
文摘Enhancing catalytic activity through modulating the interaction between N-doped carbon and metal phosphides clusters is an effective approach.Herein,the electronic structure modulation of CoP_(2) supported N-modified carbon(CoP_(2)/NC)has been designed and prepared as efficient electrocatalysts for oxygen reduction reaction(ORR),oxygen evolution reaction(OER),and hydrogen evolution reaction(HER).Notably,CoP_(2)/NC-1 catalyst exhibits impressive performance in alkaline media,with an ORR half-wave potential of 0.84 V,as well as OER and HER overpotentials of 290 and 129 mV(at 10 mA·cm^(−2)),respectively.In addition,CoP_(2)/NC-1 produces a power density as high as 172.9 mW·cm^(−2),and excellent reversibility of 100 h at 20 mA·cm^(−2) in home-made Zn-air batteries.The experimental results demonstrate that the synergistic interactions between N modified carbon substrate and CoP_(2) material significantly enhance the kinetics of ORR,OER,and HER.Density functional theory(DFT)calculations reveal the strong electrons redistribution of CoP_(2) induced by high-density N atoms at the interface,thus optimizing the key intermediates and significantly lower the energy barrier of reactions.These electronic adjustments of CoP_(2) greatly enhance its kinetics of ORR/OER/HER,leading to faster reactions.This study provides profound insights into the specific modification of CoP_(2) by N-doped carbon,enabling the construction of efficient catalysts.
基金supported by the National Natural Science Foundation of China (Grant Nos. 11474137 and 11674143)Program for Changjiang Scholars and Innovative Research Team in University (IRT 16R35)+1 种基金the Fundamental Research Funds for the Central Universities (Grant Nos. LZUMMM2018017, lzujbky-2018-121)the support of Ministry of Education (MOE2016-T2-2-138,Singapore),for research conducted at the National University of Singapore
文摘The development of e cient earth-abundant electrocatalysts for oxygen reduction, oxygen evolution, and hydrogen evolution reactions(ORR, OER, and HER) is important for future energy conversion and energy storage devices, for which both rechargeable Zn–air batteries and water splitting have raised great expectations. Herein, we report a single-phase bimetallic nickel cobalt sulfide((Ni,Co)S_2) as an e cient electrocatalyst for both OER and ORR. Owing to the synergistic combination of Ni and Co, the(Ni,Co)S_2 exhibits superior electrocatalytic performance for ORR, OER, and HER in an alkaline electrolyte, and the first principle calculation results indicate that the reaction of an adsorbed O atom with a H_2O molecule to form a *OOH is the potential limiting step in the OER. Importantly, it could be utilized as an advanced air electrode material in Zn–air batteries, which shows an enhanced charge–discharge performance(charging voltage of 1.71 V and discharge voltage of 1.26 V at 2 mA cm^(-2)), large specific capacity(842 mAh g_(Zn)^(-1) at 5 mA cm^(-2)), and excellent cycling stability(480 h). Interestingly, the(Ni,Co)S_2-based Zn–air battery can e ciently power an electrochemical water-splitting unit with(Ni,Co)S_2 serving as both the electrodes. This reveals that the prepared(Ni,Co)S_2 has promising applications in future energy conversion and energy storage devices.
基金supported by National Natural Science Foundation of China (NSFC) under Grants No. 51407020National Key Technology Research and Development Program of the Ministry of Science and Technology of China under Grants No. 2014BAC13B05Visiting Scholarship of State Key Laboratory of Power Transmission Equipment & System Security and New Technology (Chongqing University) No. 2007DA10512716404
文摘In order to investigate whether an air–water plasma jet is beneficial to improve the efficiency of inactivation, a series of experiments were done using a ring-needle plasma jet. The water content in the working gas（air） was accurately measured based on the Karl Fischer method. The effects of water on the production of OH（A;Σ;–X;Π;） and O（3p;P–3s;S） were also studied by optical emission spectroscopy. The results show that the water content is in the range of 2.53–9.58 mg l;, depending on the gas/water mixture ratio. The production of OH（A;Σ;–X;Π;） rises with the increase of water content, whereas the O（3p;P–3s;S） shows a declining tendency with higher water content. The sterilization experiments indicate that this air–water plasma jet inactivates the P. digitatum spores very effectively and its efficiency rises with the increase of the water content. It is possible that OH（A;Σ;–X;Π;） is a more effective species in inactivation than O（3p;P–3s;S） and the water content benefit the spore germination inhibition through rising the OH（A;Σ;–X;Π;） production. The maximum of the inactivation efficacy is up to 93% when the applied voltage is -6.75 kV and the water content is 9.58 mg l;.
