Splitting water under large current density is essential for efficient large-scale production and commercial utilization of hydrogen.However,the performance of the available electrocatalysts for hydrogen evolution rea...Splitting water under large current density is essential for efficient large-scale production and commercial utilization of hydrogen.However,the performance of the available electrocatalysts for hydrogen evolution reaction(HER)is far from satisfactory under large current density in alkaline electrolyte.Here we report a remarkably active and durable electrocatalyst,long and dense MoS2/Ni3S2 co-axial heterostructure nanowires on nickel foam(NF).Notably,it requires only 182 and 200 mV overpotential to achieve large current density of 500 and 1000 mA cm^-2,respectively,in alkaline solution,which are far superior to those of Pt/C-NF(281 and 444 mV)and the reported best non-noble metal catalysts(191 and 220 mV).The physical origin for this extraordinary HER performance is analyzed,which provides a useful guide for structure design of electrocatalysts to further improve their performance.展开更多
Plasma electrolytic oxidation(PEO) processes were carried out to produce ceramic layers on 6061 aluminum substrates in four kinds of electrolytes such as silicate and aluminate solution with and without sodium fluoros...Plasma electrolytic oxidation(PEO) processes were carried out to produce ceramic layers on 6061 aluminum substrates in four kinds of electrolytes such as silicate and aluminate solution with and without sodium fluorosilicate.The PEO processes were carried out under a hybrid voltage(260 V DC combined with 200 V,60 Hz AC amplitude) at room temperature for 5 min.The composition,microstructure and element distribution analyses of the PEO-treated layers were carried out by XRD and SEM & EDS.The effect of the electrolyte contents on the growth mechanism,element distribution and properties of oxide layers were studied.It is obvious that the layers generated in aluminate solutions show smoother surfaces than those in silicate solutions.Moreover,an addition of fluorine ion can effectively control the layer porosity;therefore,it can enhance the properties of the layers.展开更多
Electrochemical water splitting powered by renewables-generated electricity represents a promising approach for green hydrogen production.However,the sluggish kinetics for the hydrogen evolution reaction(HER)under an ...Electrochemical water splitting powered by renewables-generated electricity represents a promising approach for green hydrogen production.However,the sluggish kinetics for the hydrogen evolution reaction(HER)under an alkaline medium causes a massive amount of energy losses,hindering large-scale production.Exploring efficient and low-cost catalyst candidates for large-scale H_(2) generation becomes a crucial demand.Single-atom catalysts(SACs)demonstrate great promise for enabling efficient alkaline HER catalysis at maximum atom utilization efficiency.In this review,we provide a comprehensive overview of the recent progress in SACs for the HER application in alkaline environments.The fundamentals of alkaline HER are first introduced,followed by a justification of the need to develop SACs.The rational design of the SACs including the inherent element property,coordination environment,SAC morphology,and SAC mass loading are highlighted.To facilitate the development of SACs for alkaline HER,we further propose the remaining challenges and perspectives in this research field.展开更多
Electrocatalytic reduction of nitrate(NO_(3)^(−))and nitride(NO_(2)^(−))to ammonia(NH3)is of wide interest as a promising alternative to the energy-intensive Haber-Bosch route for mitigating the vast energy consumptio...Electrocatalytic reduction of nitrate(NO_(3)^(−))and nitride(NO_(2)^(−))to ammonia(NH3)is of wide interest as a promising alternative to the energy-intensive Haber-Bosch route for mitigating the vast energy consumption and the accompanied carbon dioxide emission,as well as benefiting for the relevant sewage treatment.However,exploring an efficient and low-cost catalyst with high atomic utilization that can effectively facilitate the slow multi-electron transfer process remains a grand challenge.Herein,we present an efficient hydrogenation of NO_(3)^(−)/NO_(2)^(−)species to NH3 in both alkaline and neutral environments over the Fe_(2)(MoO_(4))_(3)derived hybrid electrocatalyst with the metallic Fe site on FeMoO_(4)(Fe/FeMoO_(4)).The Mo ingredient can play a synergistically positive role in further promoting the NH_(3) production on Fe.As a result,Fe/FeMoO_(4)behaves well in the electrochemical NH_(3) generation from NO_(2)^(−)with a maximum NH_(3) Faradaic efficiency(FE)of 96.53%and 87.68%in alkaline and neutral electrolyte,corresponding to the NH_(3) yield rate of 640.68 and 302.56 mg·h^(−1)·mg_(cat.)^(−1),respectively,which outperforms the Fe and Mo counterpart and other similar catalyst,showing the robust catalytic capacity of each active site.展开更多
The severe dendrite growth on zinc anode in alkaline electrolyte brings great challenge to the development of zinc-based batteries.It is a simple and effective strategy to inhibit zinc dendrite formation by introducin...The severe dendrite growth on zinc anode in alkaline electrolyte brings great challenge to the development of zinc-based batteries.It is a simple and effective strategy to inhibit zinc dendrite formation by introducing additives into the electrolyte.In this study,N,S-doped carbon dots(TU-CQDs)were synthesized and used as additives to regulate zinc deposition in a typical KOH electrolyte.The experimental and three-dimensional transient nucleation model disclosed that the special functional groups of carbon dots can change the electrode surface state and the coordination behaviors of zinc species in the electrolyte.Therefore,TU-CQDs can not only inhibit the hydrogen evolution reaction,but also achieve uniform zinc deposition.The in-situ synchrotron radiation X-ray imaging elucidated that TU-CQDs can effectively inhibit the dendrite growth and improve the reversibility of zinc plating/stripping process.This work provides a feasible route for regulating the reversibility of zinc metal anode in alkaline electrolyte.展开更多
水系金属空气电池具有理论能量密度高、安全性高等优点,但受限于金属阳极(如锌、铁、铝、镁)的电化学不可逆性以及碱性电解质对大气中二氧化碳的化学不稳定性.本工作首次设计了一种可充电的铋-空气电池,该电池使用了非碱性的三氟甲磺酸...水系金属空气电池具有理论能量密度高、安全性高等优点,但受限于金属阳极(如锌、铁、铝、镁)的电化学不可逆性以及碱性电解质对大气中二氧化碳的化学不稳定性.本工作首次设计了一种可充电的铋-空气电池,该电池使用了非碱性的三氟甲磺酸铋(Bi(OTf)_(3))水系电解质.得益于三电子反应和相对于标准氢电极+0.32 V的高电位,铋金属负极具有383 mA h g^(−1)的高比容量和1000次循环的良好稳定性,以及99.6%高库仑效率.铋金属负极在Bi(OTf)_(3)电解液中无腐蚀、钝化和析氢等副反应.此外,非碱性的铋-空气电池通过三氧化二铋(Bi_(2)O_(3))的可逆形成/分解,在环境空气中实现了长期运行稳定性(>200 h).这项工作为探索新型水系金属空气电池作为安全稳定的电源系统提供了新思路.展开更多
Hydrogel-based quasi-solid-state electrolytes(Q-SSEs) swollen with electrolyte solutions are important components in stretchable supercapacitors and other wearable devices. This work fabricates a supertough, fatigue-r...Hydrogel-based quasi-solid-state electrolytes(Q-SSEs) swollen with electrolyte solutions are important components in stretchable supercapacitors and other wearable devices. This work fabricates a supertough, fatigue-resistant, and alkali-resistant multi-bond network(MBN) hydrogel aiming to be an alkaline Q-SSE. To synthesize the hydrogel, a 2-ureido-4[1H]-pyrimidone(UPy) motif is introduced into a poly(acrylic acid) polymer chain. The obtained MBN hydrogels with 75 wt% water content exhibit tensile strength as high as 2.47 MPa, which is enabled by the large energy dissipation ability originated from the dissociation of UPy dimers due to their high bond association energy. Owing to the high dimerization constant of UPy motifs, the dissociated UPy motifs are able to partially re-associate soon after being released from external forces, resulting in excellent fatigue-resistance. More importantly, the MBN hydrogels exhibit excellent alkali-resistance ability. The UPy Gel-10 swollen with 1 mol/L KOH display a tensile strength as high as ~1.0 MPa with elongation at break of ~550%. At the same time, they show ionic conductivity of ~17 m S/cm, which do not decline even when the hydrogels are stretched to 500% strain.The excellent mechanical property and ionic conductivity of the present hydrogels demonstrate potential application as a stretchable alkaline Q-SSE.展开更多
基金supported by the National Natural Science Foundation of China(51325205,51290273,51521091,and 51861135201)the Chinese Academy of Sciences(XDB30000000,and ZDBS-LY-JSC027)+2 种基金Liaoning Revitalization Talents Program(XLYC1808013)the Program for Guangdong Introducing Innovative and Enterpreneurial Teams(2017ZT07C341)the Development and Reform Commission of Shenzhen Municipality for the development of the“Low-Dimensional Materials and Devices”discipline,and the Economic,Trade and Information Commission of Shenzhen Municipality for the“2017 Graphene Manufacturing Innovation Center Project”(201901171523).
文摘Splitting water under large current density is essential for efficient large-scale production and commercial utilization of hydrogen.However,the performance of the available electrocatalysts for hydrogen evolution reaction(HER)is far from satisfactory under large current density in alkaline electrolyte.Here we report a remarkably active and durable electrocatalyst,long and dense MoS2/Ni3S2 co-axial heterostructure nanowires on nickel foam(NF).Notably,it requires only 182 and 200 mV overpotential to achieve large current density of 500 and 1000 mA cm^-2,respectively,in alkaline solution,which are far superior to those of Pt/C-NF(281 and 444 mV)and the reported best non-noble metal catalysts(191 and 220 mV).The physical origin for this extraordinary HER performance is analyzed,which provides a useful guide for structure design of electrocatalysts to further improve their performance.
基金Korea Research Foundation Grant (KRF-2006-005-J02703)
文摘Plasma electrolytic oxidation(PEO) processes were carried out to produce ceramic layers on 6061 aluminum substrates in four kinds of electrolytes such as silicate and aluminate solution with and without sodium fluorosilicate.The PEO processes were carried out under a hybrid voltage(260 V DC combined with 200 V,60 Hz AC amplitude) at room temperature for 5 min.The composition,microstructure and element distribution analyses of the PEO-treated layers were carried out by XRD and SEM & EDS.The effect of the electrolyte contents on the growth mechanism,element distribution and properties of oxide layers were studied.It is obvious that the layers generated in aluminate solutions show smoother surfaces than those in silicate solutions.Moreover,an addition of fluorine ion can effectively control the layer porosity;therefore,it can enhance the properties of the layers.
基金This work was sup-ported by the Australian Research Council Discovery Projects(Grant Nos.ARC DP200103332 and ARC DP200103315)。
文摘Electrochemical water splitting powered by renewables-generated electricity represents a promising approach for green hydrogen production.However,the sluggish kinetics for the hydrogen evolution reaction(HER)under an alkaline medium causes a massive amount of energy losses,hindering large-scale production.Exploring efficient and low-cost catalyst candidates for large-scale H_(2) generation becomes a crucial demand.Single-atom catalysts(SACs)demonstrate great promise for enabling efficient alkaline HER catalysis at maximum atom utilization efficiency.In this review,we provide a comprehensive overview of the recent progress in SACs for the HER application in alkaline environments.The fundamentals of alkaline HER are first introduced,followed by a justification of the need to develop SACs.The rational design of the SACs including the inherent element property,coordination environment,SAC morphology,and SAC mass loading are highlighted.To facilitate the development of SACs for alkaline HER,we further propose the remaining challenges and perspectives in this research field.
基金supported in part by the National Natural Science Foundation of China(Nos.51925102 and 52273277)H.-X.Z.acknowledges funding from the National Natural Science Foundation of China Outstanding Youth Science Foundation of China(Overseas).
文摘Electrocatalytic reduction of nitrate(NO_(3)^(−))and nitride(NO_(2)^(−))to ammonia(NH3)is of wide interest as a promising alternative to the energy-intensive Haber-Bosch route for mitigating the vast energy consumption and the accompanied carbon dioxide emission,as well as benefiting for the relevant sewage treatment.However,exploring an efficient and low-cost catalyst with high atomic utilization that can effectively facilitate the slow multi-electron transfer process remains a grand challenge.Herein,we present an efficient hydrogenation of NO_(3)^(−)/NO_(2)^(−)species to NH3 in both alkaline and neutral environments over the Fe_(2)(MoO_(4))_(3)derived hybrid electrocatalyst with the metallic Fe site on FeMoO_(4)(Fe/FeMoO_(4)).The Mo ingredient can play a synergistically positive role in further promoting the NH_(3) production on Fe.As a result,Fe/FeMoO_(4)behaves well in the electrochemical NH_(3) generation from NO_(2)^(−)with a maximum NH_(3) Faradaic efficiency(FE)of 96.53%and 87.68%in alkaline and neutral electrolyte,corresponding to the NH_(3) yield rate of 640.68 and 302.56 mg·h^(−1)·mg_(cat.)^(−1),respectively,which outperforms the Fe and Mo counterpart and other similar catalyst,showing the robust catalytic capacity of each active site.
基金financially supported by the National Key Research and Development Program of China(No.2019YFC1907801)Innovation-Driven Project of Central South University(No.2020CX007).
文摘The severe dendrite growth on zinc anode in alkaline electrolyte brings great challenge to the development of zinc-based batteries.It is a simple and effective strategy to inhibit zinc dendrite formation by introducing additives into the electrolyte.In this study,N,S-doped carbon dots(TU-CQDs)were synthesized and used as additives to regulate zinc deposition in a typical KOH electrolyte.The experimental and three-dimensional transient nucleation model disclosed that the special functional groups of carbon dots can change the electrode surface state and the coordination behaviors of zinc species in the electrolyte.Therefore,TU-CQDs can not only inhibit the hydrogen evolution reaction,but also achieve uniform zinc deposition.The in-situ synchrotron radiation X-ray imaging elucidated that TU-CQDs can effectively inhibit the dendrite growth and improve the reversibility of zinc plating/stripping process.This work provides a feasible route for regulating the reversibility of zinc metal anode in alkaline electrolyte.
基金financially supported by the Science and Technology Commission of Shanghai Municipality(STCSM,21511104900 and 20JC1414902)the National Natural Science Foundation of China(52222310).
文摘水系金属空气电池具有理论能量密度高、安全性高等优点,但受限于金属阳极(如锌、铁、铝、镁)的电化学不可逆性以及碱性电解质对大气中二氧化碳的化学不稳定性.本工作首次设计了一种可充电的铋-空气电池,该电池使用了非碱性的三氟甲磺酸铋(Bi(OTf)_(3))水系电解质.得益于三电子反应和相对于标准氢电极+0.32 V的高电位,铋金属负极具有383 mA h g^(−1)的高比容量和1000次循环的良好稳定性,以及99.6%高库仑效率.铋金属负极在Bi(OTf)_(3)电解液中无腐蚀、钝化和析氢等副反应.此外,非碱性的铋-空气电池通过三氧化二铋(Bi_(2)O_(3))的可逆形成/分解,在环境空气中实现了长期运行稳定性(>200 h).这项工作为探索新型水系金属空气电池作为安全稳定的电源系统提供了新思路.
基金the National Natural Science Foundation of China (Nos. 21774069, 51633003 and 21474058) for financial support。
文摘Hydrogel-based quasi-solid-state electrolytes(Q-SSEs) swollen with electrolyte solutions are important components in stretchable supercapacitors and other wearable devices. This work fabricates a supertough, fatigue-resistant, and alkali-resistant multi-bond network(MBN) hydrogel aiming to be an alkaline Q-SSE. To synthesize the hydrogel, a 2-ureido-4[1H]-pyrimidone(UPy) motif is introduced into a poly(acrylic acid) polymer chain. The obtained MBN hydrogels with 75 wt% water content exhibit tensile strength as high as 2.47 MPa, which is enabled by the large energy dissipation ability originated from the dissociation of UPy dimers due to their high bond association energy. Owing to the high dimerization constant of UPy motifs, the dissociated UPy motifs are able to partially re-associate soon after being released from external forces, resulting in excellent fatigue-resistance. More importantly, the MBN hydrogels exhibit excellent alkali-resistance ability. The UPy Gel-10 swollen with 1 mol/L KOH display a tensile strength as high as ~1.0 MPa with elongation at break of ~550%. At the same time, they show ionic conductivity of ~17 m S/cm, which do not decline even when the hydrogels are stretched to 500% strain.The excellent mechanical property and ionic conductivity of the present hydrogels demonstrate potential application as a stretchable alkaline Q-SSE.
