For treatment of sulfion-containing wastewater,coupling the electrochemical sulfion oxidation reaction(SOR)with hydrogen evolution reaction(HER)can be an ideal way for sulfur and H_(2)resources recovery.Herein,we synt...For treatment of sulfion-containing wastewater,coupling the electrochemical sulfion oxidation reaction(SOR)with hydrogen evolution reaction(HER)can be an ideal way for sulfur and H_(2)resources recovery.Herein,we synthesize a metal-modified carbon nanotube arrays electrode(Co@N-CNTs/CC)for SOR and HER.This electrode has excellent performance for SOR and HER attributed to the unique array structure.It can achieve 99.36 mA/cm^(2)at 0.6 V for SOR,and 10 mA/cm^(2)at 0.067 V for HER.Density functional theory calculations verify that metal modification is able to regulate the electronic structure of carbon nanotube,which is able to optimize the adsorption of intermediates.Employed Co@N-CNTs/CC as bifunctional elec-trodes to establish a hybrid electrolytic cell can reduce about 67%of energy consumption compared with the traditional water splitting electrolytic cell.Finally,the hybrid electrolytic cell is used to treat actual sulfion-containing wastewater,achieving the sulfur yield of 30 mg h^(−1)cm^(−2)and the hydrogen production of 0.64 mL/min.展开更多
本文通过微波法超快速制备了泡沫镍(NF)负载的Co/Zn复合氧化物(Co-Zn/NF)。XRD测试表明生成的Co/Zn复合氧化物具有低结晶度。采用线性扫描伏安法(LSV)测试了Co-Zn/NF在碱性条件下的电催化硫离子氧化性能。与泡沫镍负载的单金属氧化物(Co...本文通过微波法超快速制备了泡沫镍(NF)负载的Co/Zn复合氧化物(Co-Zn/NF)。XRD测试表明生成的Co/Zn复合氧化物具有低结晶度。采用线性扫描伏安法(LSV)测试了Co-Zn/NF在碱性条件下的电催化硫离子氧化性能。与泡沫镍负载的单金属氧化物(Co/NF和Zn/NF)相比,Co-Zn/NF表现出更好的催化性能。在含有1 mol·L^(-1)Na2S和1 mol·L^(-1)NaOH的电解液中,Co-Zn/NF达到100 m A·cm^(-2)的电流密度所需的电位仅为0.28 V vs RHE,并且在恒定100 m A·cm^(-2)的电流密度下,长时间工作35小时后仍保持高的催化性能。此外,组装非对称电解槽(阳极:硫离子氧化反应(sulfion oxidation reaction,SOR)用1 mol·L^(-1)Na2S和1mol·L^(-1)NaOH为电解质,阴极:析氢反应(hydrogen evolution reaction,HER)用1 mol·L^(-1)Na OH为电解质)进行双电极硫氧化辅助电解水制氢测试,与传统的碱性电解水相比,达到100 m A·cm^(-2)电流密度所需的能耗降低了46%。本工作为低能耗电化学制氢提供了一种新思路,并证明了SOR耦合HER电解水制氢具有实际应用的可行性。展开更多
基金supported by Natural Science Foundation of Shandong Province(Nos.ZR2022QE076,ZR2021JQ15,ZR2019YQ20)the National Natural Science Foundation of China(Nos.52002145,52202092,51972147,52022037)Taishan Scholars Project Special Funds(No.tsqn201812083).
文摘For treatment of sulfion-containing wastewater,coupling the electrochemical sulfion oxidation reaction(SOR)with hydrogen evolution reaction(HER)can be an ideal way for sulfur and H_(2)resources recovery.Herein,we synthesize a metal-modified carbon nanotube arrays electrode(Co@N-CNTs/CC)for SOR and HER.This electrode has excellent performance for SOR and HER attributed to the unique array structure.It can achieve 99.36 mA/cm^(2)at 0.6 V for SOR,and 10 mA/cm^(2)at 0.067 V for HER.Density functional theory calculations verify that metal modification is able to regulate the electronic structure of carbon nanotube,which is able to optimize the adsorption of intermediates.Employed Co@N-CNTs/CC as bifunctional elec-trodes to establish a hybrid electrolytic cell can reduce about 67%of energy consumption compared with the traditional water splitting electrolytic cell.Finally,the hybrid electrolytic cell is used to treat actual sulfion-containing wastewater,achieving the sulfur yield of 30 mg h^(−1)cm^(−2)and the hydrogen production of 0.64 mL/min.
文摘本文通过微波法超快速制备了泡沫镍(NF)负载的Co/Zn复合氧化物(Co-Zn/NF)。XRD测试表明生成的Co/Zn复合氧化物具有低结晶度。采用线性扫描伏安法(LSV)测试了Co-Zn/NF在碱性条件下的电催化硫离子氧化性能。与泡沫镍负载的单金属氧化物(Co/NF和Zn/NF)相比,Co-Zn/NF表现出更好的催化性能。在含有1 mol·L^(-1)Na2S和1 mol·L^(-1)NaOH的电解液中,Co-Zn/NF达到100 m A·cm^(-2)的电流密度所需的电位仅为0.28 V vs RHE,并且在恒定100 m A·cm^(-2)的电流密度下,长时间工作35小时后仍保持高的催化性能。此外,组装非对称电解槽(阳极:硫离子氧化反应(sulfion oxidation reaction,SOR)用1 mol·L^(-1)Na2S和1mol·L^(-1)NaOH为电解质,阴极:析氢反应(hydrogen evolution reaction,HER)用1 mol·L^(-1)Na OH为电解质)进行双电极硫氧化辅助电解水制氢测试,与传统的碱性电解水相比,达到100 m A·cm^(-2)电流密度所需的能耗降低了46%。本工作为低能耗电化学制氢提供了一种新思路,并证明了SOR耦合HER电解水制氢具有实际应用的可行性。
