Deactivation mechanism for water splitting:Recent advances

Hydrogen(H_(2)) has been regarded as a promising alternative to fossil-fuel energy.Green H_(2) produced via water electrolysis(WE)powered by renewable energy could achieve a zero-carbon footprint.Considerable attention has been focused on developing highly active catalysts to facilitate the reaction kinetics and improve the energy efficiency of WE.However,the stability of the electrocatalysts hampers the commercial viability of WE.Few studies have elucidated the origin of catalyst degradation.In this review,we first discuss the WE mechanism,including anodic oxygen evolution reaction(OER)and cathodic hydrogen evolution reaction(HER).Then,we provide strategies used to enhance the stability of electrocatalysts.After that,the deactivation mechanisms of the typical commercialized HER and OER catalysts,including Pt,Ni,RuO_(2),and IrO_(2),are summarized.Finally,the influence of fluctuating energy on catalyst degradation is highlighted and in situ characterization methodologies for understanding the dynamic deactivation processes are described.

Single-atomic tungsten-doped Co_(3)O_(4) nanosheets for enhanced electrochemical kinetics in lithium–sulfur batteries

The practical application of lithium–sulfur batteries(LSBs)is severely hindered by the undesirable shuttling of lithium polysulfides(LiPSs)and sluggish redox kinetics of sulfur species.Herein,a series of ultrathin singleatomic tungsten-doped Co_(3)O_(4)(Wx-Co_(3)O_(4))nanosheets as catalytic additives in the sulfur cathode for LSBs are rationally designed and synthesized.Benefiting from the enhanced catalytic activity and optimized electronic structure by W doping,the Wx-Co_(3)O_(4) not only reduces the shuttling of LiPSs but also decreases the energy barrier of sulfur redox reactions of sulfur species,leading to accelerated electrode kinetic.As a result,LSB cathodes with the use of 5.0 wt%W0.02-Co_(3)O_(4) as the electrocatalyst show the high reversible capacities of 1217.0 and 558.6 mAh g^(-1) at 0.2 and 5.0 C,respectively,and maintain a high reversible capacity of 644.6 mAh g^(-1) at 1.0 C(1.0 C=1675 mA g^(-1))after 500 cycles.With a high sulfur loading of 5.5 mg cm^(-2) and electrolyte–electrode ratio of 8μL_(electrolyte) mg_(sulfur)^(-1),the 5.0 wt%W_(0.02)-Co_(3)O_(4)-based sulfur cathode also retains a high reversible areal capacity of 3.86 mAh cm^(-2) at 0.1 C after 50 cycles with an initial capacity retention of 84.7%.

Interface Engineering of CoS/CoO@N‑Doped Graphene Nanocomposite for High‑Performance Rechargeable Zn–Air Batteries

Low cost and green fabrication of high-performance electrocatalysts with earth-abundant resources for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)are crucial for the large-scale application of rechargeable Zn-air batteries(ZABs).In this work,our density functional theory calculations on the electrocatalyst suggest that the rational construction of interfacial structure can induce local charge redistribution,improve the electronic conductivity and enhance the catalyst stability.In order to realize such a structure,we spatially immobilize heterogeneous CoS/CoO nanocrystals onto N-doped graphene to synthesize a bifunctional electrocatalyst(CoS/CoO@NGNs).The optimization of the composition,interfacial structure and conductivity of the electrocatalyst is conducted to achieve bifunctional catalytic activity and deliver outstanding efficiency and stability for both ORR and OER.The aqueous ZAB with the as-prepared CoS/CoO@NGNs cathode displays a high maximum power density of 137.8 mW cm^−2,a specific capacity of 723.9 mAh g^−1 and excellent cycling stability(continuous operating for 100 h)with a high round-trip efficiency.In addition,the assembled quasi-solid-state ZAB also exhibits outstanding mechanical flexibility besides high battery performances,showing great potential for applications in flexible and wearable electronic devices.

Cobalt-doped Mn3O4 nanocrystals embedded in graphene nanosheets as a high-performance bifunctional oxygen electrocatalyst for rechargeable Zn–Air batteries

A non-noble-metal bifunctional catalyst with efficient and durable activity towards both the oxygen reduction reaction(ORR)and the oxygen evolution reaction(OER)is crucial to the development of rechargeable Zn-air batteries.Herein,a facile one-step hydrothermal method is reported for the synthesis of a high-performance bifunctional oxygen electrocatalyst,cobalt-doped Mn_(3)O_(4) nanocrystals supported on graphene nanosheets(Co–Mn_(3)O_(4)/G).Compare to pristine Mn_(3)O_(4),this Co–Mn_(3)O_(4)/G exhibits greatly enhanced electrocatalytic activity,delivering a halfwave potential of 0.866 V for the ORR and a low overpotential of 275 mV at 10 mA cm^(-2) for the OER.The zinc-air battery built with Co–Mn_(3)O_(4)/G shows a reduced charge–discharge voltage of 0.91 V at 10 mA cm^(-2),an power density of 115.24 mW cm^(-2) and excellent stability without any degradation after 945 cycles(315 h),outperforming the state-of-the-art Pt/C–Ir/C catalyst-based device.

Cation-vacancy induced Li+ intercalation pseudocapacitance at atomically thin heterointerface for high capacity and high power lithium-ion batteries

It is challenging to create cation vacancies in electrode materials for enhancing the performance of rechargeable lithium ion batteries (LIBs). Herein, we utilized a strong alkaline etching method to successfully create Co vacancies at the interface of atomically thin Co_(3−x)O_(4)/graphene@CNT heterostructure for high-energy/power lithium storage. The creation of Co-vacancies in the sample was confirmed by high-resolution scanning transmission electron microscope (HRSTEM), X-ray photoelectron spectroscopy (XPS) and electron energy loss near-edge structures (ELNES). The obtained Co_(3−x)O_(4)/graphene@CNT delivers an ultra-high capacity of 1688.2 mAh g^(−1) at 0.2 C, excellent rate capability of 83.7% capacity retention at 1 C, and an ultralong life up to 1500 cycles with a reversible capacity of 1066.3 mAh g^(−1). Reaction kinetic study suggests a significant contribution from pseudocapacitive storage induced by the Co-vacancies at the Co_(3−x)O_(4)/graphene@CNT interface. Density functional theory confirms that the Co-vacancies could dramatically enhance the Li adsorption and provide an additional pathway with a lower energy barrier for Li diffusion, which results in an intercalation pseudocapacitive behavior and high-capacity/rate energy storage.

Correction to:Interface Engineering of CoS/CoO@N-Doped Graphene Nanocomposite for High-Performance Rechargeable Zn-Air Batteries

In the original publication,the label text“Pt/C”in Fig.5 should be“Pt/C+IrO_(2)”.In Fig.5d,the X-axis label“Poten-tial(V vs.RHE)”should be replaced with“Specific capacity(mAh g^(−1))”.In Fig.5e,the Y-axis label“Potential(V vs.RHE)”should be replaced with“Voltage(V)”.In Fig.5g,the X-axis label“Time(h)”should be replaced with“Cycle number(n)”.The Y-axis label“ΔE(V vs.RHE)”should be replaced with“Voltage(V)”.The number“1.4”and“1.6”should be replaced with 1.6 and 2.0,respectively.The cor-responding data analysis and conclusions in the manuscript are not affected and thus not to be changed.The correct Fig.5 is provided in this correction.

Corrigendum to“Cation-vacancy induced Li+intercalation pseudocapacitance at atomically thin heterointerface for high capacity and high power lithium-ion batteries”[J.Energy Chem.62(2021)281–288]

The authors regret that the wrong image of Fig.1 was uploaded in the paper.The correct one should be:We confirm the discrepancy is restricted to the image of Fig.1 only,the underlying data is correct and unchanged.The authors would like to apologise for any inconvenience caused.

2020 roadmap on pore materials for energy and environmental applications

Porous materials have attracted great attention in energy and environment applications,such as metal organic frameworks(MOFs),metal aerogels,carbon aerogels,porous metal oxides.These materials could be also hybridized with other materials into functional composites with superior properties.The high specific area of porous materials offer them the advantage as hosts to conduct catalytic and electrochemical reactions.On one hand,catalytic reactions include photocatalytic,p ho toe lectrocatalytic and electrocatalytic reactions over some gases.On the other hand,they can be used as electrodes in various batteries,such as alkaline metal ion batteries and electrochemical capacitors.So far,both catalysis and batteries are extremely attractive topics.There are also many obstacles to overcome in the exploration of these porous materials.The research related to porous materials for energy and environment applications is at extremely active stage,and this has motivated us to contribute with a roadmap on ’porous materials for energy and environment applications’.

Understanding of the capacity Contribution of carbon in phosphorus-carbon composites for high-performance anodes in lithium ion batteries

Phosphorus has recently received extensive attention as a promising anode for lithium ion batteries （LIBs） due to its high theoretical capacity of 2,596 mAh·g^-1. To develop high-performance phosphorus anodes for LIBs, carbon materials have been hybridized with phosphorus （P-C） to improve dispersion and con- ductivity. However, the specific capacity, rate capability, and cycling stability of P-C anodes are still less than satisfactory for practical applications. Furthermore, the exact effects of the carbon support on the electrochemical performance of the P-C anodes are not fully understood. Herein, a series of xP-yC anode materials for LIBs were prepared by a simple and efficient ball-milling method. 6P-4C and 3P-7C were found to be optimum mass ratios of x/y, and delivered initial discharge capacities of 1,803.5 and 1,585.3-mAh·g^-1, respectively, at 0.1 C in the voltage range 0.02-2 V, with an initial capacity retention of 68.3% over 200 cycles （more than 4 months cycling life） and 40.8% over 450 cycles. The excellent electrochemical performance of the 6P-4C and 3P-7C samples was attributed to a synergistic effect from both the adsorbed P and carbon.

Pulse-potential electrochemistry to boost real-life application of pseudocapacitive dual-doped polypyrrole

Polypyrrole(PPy)is a very promising pseudocapacitive electrode material for supercapacitors.However,the poor electrochemical performances and cycling stability caused by volumetric change and counterion drain severely limited its practical application and commercialization.Herein,we present a pulsepotential polymerization strategy for uniformly depositing a dual-doped PPy with ordered and shorter molecular structure by balancing the concentration polarization.Such a strategy ensures more homogeneous stress distribution of PPy during ultralong cycling tests and improves the cycle stability.Moreover,the pulse-potential polymerized PPy with dual anion doping behavior induces enhanced protonation level and improved electrical conductivity,which boosting the charge transfer kinetics.Therefore,the as-synthesized PPy exhibits a remarkable capacitance performance(7250 mF/cm^(2)@3 mA/cm^(2)),outstanding rate capability(3073 mF/cm^(2)@200 mA/cm^(2))and a long cycle life.The assembled symmetric and asymmetric supercapacitors(ASC)exhibit good energy densities(0.8 mWh/cm^(2) for ASC and 0.5 mWh/cm^(2) for symmetric supercapacitor),and excellent durability with zero capacitive loss after 35,000 cycles.In addition,we have fabricated small pouch devices,which can effectively operate a variety of electronic products(including the high-voltage 5 V smartphone,and tablet)and well withstand the external extreme tests during operation,demonstrating the quantitative investigation of the real-life application of aqueous supercapacitors.