High-rate electrochemical H_(2)O_(2) production over multimetallic atom catalysts under acidic–neutral conditions

Hydrogen peroxide(H_(2)O_(2))production by the electrochemical 2-electron oxygen reduction reaction(2e−ORR)is a promising alternative to the energy-intensive anthraquinone process,and single-atom electrocatalysts show the unique capability of high selectivity toward 2e−ORR against the 4e−one.The extremely low surface density of the single-atom sites and the inflexibility in manipulating their geometric/electronic configurations,however,compromise the H_(2)O_(2) yield and impede further performance enhancement.Herein,we construct a family of multiatom catalysts(MACs),on which two or three single atoms are closely coordinated to form high-density active sites that are versatile in their atomic configurations for optimal adsorption of essential*OOH species.Among them,the Cox–Ni MAC presents excellent electrocatalytic performance for 2e−ORR,in terms of its exceptionally high H_(2)O_(2) yield in acidic electrolytes(28.96 mol L^(−1) gcat.^(−1) h^(−1))and high selectivity under acidic to neutral conditions in a wide potential region(>80%,0–0.7 V).Operando X-ray absorption and density functional theory analyses jointly unveil its unique trimetallic Co2NiN8 configuration,which efficiently induces an appropriate Ni–d orbital filling and modulates the*OOH adsorption,together boosting the electrocatalytic 2e−ORR capability.This work thus provides a new MAC strategy for tuning the geometric/electronic structure of active sites for 2e−ORR and other potential electrochemical processes.

Identification of the highly active Zn-N_(4) sites with pyrrole/pyridine-N synergistic coordination by dz^(2)+s-band center for electrocatalytic H_(2)O_(2) production

Single metal atoms anchored on nitrogen-doped carbon materials(M-N_(4))have been identified as effective active sites for catalyzing the two-electron oxygen reduction reaction(2e-ORR).However,the relationship between the local atomic/electronic environments of the M-N_(4) sites(metal atoms coordinated with different types of N species)and their catalytic activity for 2e-ORR has rarely been elaborated clearly,which imposes significant ambiguity for the rational design of catalysts.Herein,guided by the comprehensive density-functional theory calculations and predictions,a series of Zn-N_(4) single-atom catalysts(SACs)are designed with pyrrole/pyridine-N(N_(Po)/N_(Pd))synergistic coordination and prepared by controlling the pyrolysis temperature(600,700,and 800℃),Among them,the dominated Zn-N_(4) configurations with rationally combined N_(Po)/N_(Pd)coordination show~*OOH adsorption strength close to the optimal value,much superior to those with mono N species.Thus,the as-prepared catalyst exhibits a high H_(2)O_(2) selectivity of over 90%both in neutral and alkaline environments,with a superb H_(2)O_(2) yield of up to 33.63 mol g^(-1)h^(-1)in an alkaline with flow cell.More importantly,a new descriptor,dz^(2)+s band center,has been proposed,which is especially feasible for predicting the activity for metal types with fully occupied s and d orbitals.This work thus presents clear guidance for the rational design of highly active SACs toward ORR and provides a complement to the d-band theory for more accurately predicting the catalytic activity of the materials.

Recent progress on the recycling technology of Li-ion batteries

Lithium-ion batteries(LIBs)have been widely applied in portable electronic devices and electric vehicles.With the booming of the respective markets,a huge quantity of spent LIBs that typically use either LiFePO_(4) or Li N_(x)Co_(y)Mn_(z)O_(2) cathode materials will be produced in the very near future,imposing significant pressure for the development of suitable disposal/recycling technologies,in terms of both environmental protection and resource reclaiming.In this review,we firstly do a comprehensive summary of the-state-of-art technologies to recycle Li N_(x)Co_(y)Mn_(z)O_(2) and LiFePO_(4)-based LIBs,in the aspects of pretreatment,hydrometallurgical recycling,and direct regeneration of the cathode materials.This closed-loop strategy for cycling cathode materials has been regarded as an ideal approach considering its economic benefit and environmental friendliness.Afterward,as for the exhausted anode materials,we focus on the utilization of exhausted anode materials to obtain other functional materials,such as graphene.Finally,the existing challenges in recycling the LiFePO_(4) and Li N_(x)Co_(y)Mn_(z)O_(2) cathodes and graphite anodes for industrial-scale application are discussed in detail;and the possible strategies for these issues are proposed.We expect this review can provide a roadmap towards better technologies for recycling LIBs,shed light on the future development of novel battery recycling technologies to promote the environmental benignity and economic viability of the battery industry and pave way for the large-scale application of LIBs in industrial fields in the near future.

A flexible carbon nanotube@V_(2)O_(5) film as a high-capacity and durable cathode for zinc ion batteries

Aqueous zinc-ion batteries(ZIBs)are receiving a continuously increasing attention for mobile devices,especially for the flexible and wearable electronics,due to their non-toxicity,non-flammability,and low-cost features.Despite the significant progress in achieving higher capacities for electrode materials of ZIBs,to endow them with high flexibility and economic feasibility is,however,still a significant challenge remaining unsolved.Herein,we present a highly flexible composite film composed of carbon nanotube film and V_(2)O_(5)(CNTF@V_(2)O_(5))with high strength and high conductivity,which is prepared by simply impregnating a porous CNT film with an aqueous V_(2)O_(5)sol under vacuum.For this material,intimate incorporation between V_(2)O_(5)and CNTs has been achieved,successfully integrating the high zinc ion storage capability with high mechanical flexibility.As a result,this CNTF@V_(2)O_(5)film delivers a high capacity of 356.6 m Ah g^(-1)at 0.4 A g^(-1)and excellent cycling stability with 80.1%capacity retention after 500 cycles at 2.0 A g^(-1).The novel strategy and the outstanding battery performance presented in this work should shed light on the development of high-performance and flexible ZIBs.

Dual-modification of manganese oxide by heterostructure and cation pre-intercalation for high-rate and stable zinc-ion storage

Zinc-ion batteries(ZIBs)possess great advantages in terms of high safety and low cost,and are regarded as promising alternatives to lithium-ion batteries(LIBs).However,limited by the electrochemical kinetics and structural stability of the typical cathode materials,it is still difficult to simultaneously achieve high rates and high cycling stability for ZIBs.Herein,we present a manganese oxide(Sn_(x)Mn O_(2)/Sn O_(2))material that is dual-modified by Sn O_(2)/Mn O_(2)heterostructures and pre-intercalated Sn;cations as the cathode material for ZIBs.Such modification provides sufficient hetero-interfaces and expanded interlayer spacing in the material,which greatly facilitates the insertion/extraction of Zn^(2+).Meanwhile,the“structural pillars”of Sn^(4+) cations and the“pinning effect”of SnO_(2)also structurally stabilizes the Mn O_(2)species during the repeated Zn^(2+) insertion/extraction,leading to ultra-high cycling stability.Due to these merits,the Sn_(x)MnO_(2)/SnO_(2)cathode exhibits a high reversible capacity of 316.1 m Ah g^(-1) at 0.3 A g^(-1),superior rate capability of 179.4 m Ah g^(-1) at 2 A g^(-1),and 92.4%capacity retention after 2000 cycles.Consequently,this work would provide a promising yet efficient strategy by combining heterostructures and cations preintercalation to obtain high-performance cathodes for ZIBs.

Multiatom activation of single-atom electrocatalysts via remote coordination for ultrahigh-rate two-electron oxygen reduction

Electrocatalytic oxygen reduction via a two-electron pathway(2e^(-)-ORR)is a promising and eco-friendly route for producing hydrogen peroxide(H_(2)O_(2)).Single-atom catalysts(SACs)typically show excellent selectivity towards 2e^(-)-ORR due to their unique electronic structures and geometrical configurations.The very low density of single-atom active centers,however,often leads to unsatisfactory H_(2)O_(2)yield rate,significantly inhibiting their practical feasibility.Addressing this,we herein introduce fluorine as a secondary doping element into conventional SACs,which does not directly coordinate with the singleatom metal centers but synergize with them in a remote manner.This strategy effectively activates the surrounding carbon atoms and converts them into highly active sites for 2e^(-)-ORR.Consequently,a record-high H_(2)O_(2)yield rate up to 27 mol g^(-1)h^(-1)has been achieved on the Mo–F–C catalyst,with high Faradaic efficiency of 90%.Density functional theory calculations further confirm the very kinetically facile 2e^(-)-ORR over these additional active sites and the superiority of Mo as the single-atom center to others.This strategy thus not only provides a high-performance electrocatalyst for 2e^(-)-ORR but also should shed light on new strategies to significantly increase the active centers number of SACs.

Graphitic carbon nitride (g-C3N4)-based nanosized heteroarrays: Promising materials for photoelectrochemical water splitting

Photoelectrochemical(PEC)water splitting is recognized as a sustainable strategy for hydrogen generation due to its abundant hydrogen source,utilization of inexhaustible solar energy,high-purity product,and environment-friendly process.To actualize a practical PEC water splitting,it is paramount to develop efficient,stable,safe,and low-cost photoelectrode materials.Recently,graphitic carbon nitride(g-C3N4)has aroused a great interest in the new generation photoelectrode materials because of its unique features,such as suitable band structure for water splitting,a certain range of visible light absorption,nontoxicity,and good stability.Some inherent defects of g-C3N4,however,seriously impair further improvement on PEC performance,including low electronic conductivity,high recombination rate of photogenerated charges,and limited visible light absorption at long wavelength range.Construction of g-C3N4-based nanosized heteroarrays as photoelectrodes has been regarded as a promising strategy to circumvent these inherent limitations and achieve the high-performance PEC water splitting due to the accelerated exciton separation and the reduced combination of photogenerated electrons/holes.Herein,we summarize in detail the latest progress of g-C3N4-based nanosized heteroarrays in PEC water-splitting photoelectrodes.Firstly,the unique advantages of this type of photoelectrodes,including the highly ordered nanoarray architectures and the heterojunctions,are highlighted.Then,different g-C3N4-based nanosized heteroarrays are comprehensively discussed,in terms of their fabrication methods,PEC capacities,and mechanisms,etc.To conclude,the key challenges and possible solutions for future development on g-C3N4-based nanosized heteroarray photoelectrodes are discussed.

Ultrathin Ni_(x)Co_(y)-silicate nanosheets natively anchored on CNTs films for flexible lithium ion batteries

The rapid development of portable and wearable electronics has called for novel flexible electrodes with superior performance.The development of flexible electrode materials with excellent mechanical and electrochemical properties has become one of the key factors for this goal.Here,a Ni_(x)Co_(y)-silicate@CNTs film is developed as a flexible anode for lithium ion batteries(LIBs).On this film,Ni_(x)Co_(y)-silicate nanosheets are firmly and intimately anchored on the surface of CNTs,which have a 3D network structure and link the adjacent nanosheets together.Benefitted from this,the composite film is not only sufficient to withstand various deformations due to its excellent flexibility but also has excellent electrochemical properties,in terms of high reversible capacity of 1047 mAh g^(-1) at 0.1 A g^(-1) as well as a high rate and cycling performance(capacity retention up to 78.13% after 140 cycles).The pouch-type full flexible LIB using this material can stably operate under various bending conditions,showing the great potential of this 3 D Ni_(x)Co_(y)-silicate@CNTs film for flexible energy storage devices with high durability.

Photoelectrochemical nitrogen reduction:A step toward achieving sustainable ammonia synthesis

Industrial NH3 production mainly employs the well‐known Haber‐Bosch(H‐B)process,which is associated with significant energy consumption and carbon emissions.Photoelectrochemical nitro‐gen reduction reaction(PEC‐NRR)under ambient conditions is considered a promising alternative to the H‐B process and has been attracting increasing attention owing to its associated energy effi‐ciency and environmentally friendly characteristics.The performance of a PEC‐NRR system,such as the NH_(3) yield,selectivity,and stability,is essentially determined by its key component,the photo‐cathode.In this review,the latest progress in the development of photocathode materials employed in PEC‐NRR is evaluated.The fundamental mechanisms and essential features required for the PEC‐NRR are introduced,followed by a discussion of various types of photocathode materials,such as oxides,sulfides,selenides,black silicon,and black phosphorus.In particular,the PEC‐NRR reac‐tion mechanisms associated with these photocathode materials are reviewed in detail.Finally,the present challenges and future opportunities related to the further development of PEC‐NRR are also discussed.This review aims to improve the understanding of PEC‐NRR photocathode materials while also shedding light on the new concepts and significant innovations in this field.

A flexible CNT@nickel silicate composite film for high-performance sodium storage

Due to the sufficient ion diffusion channels provided by the large interlayer spacing, layered silicates are widely considered as potential anode materials for lithium ion and sodium ion batteries. However, due to the poor electronic conductivity, the application of layered silicates for electrochemical energy storage has been greatly limited. Carbon nanotube(CNT) film has excellent electrical conductivity and a unique interconnected network, making it an ideal matrix for composite electrochemical material. We herein report a CNT@nickel silicate composite film(CNT@NiSiO) fabricated by a SiO2-mediated hydrothermal conversion process, for sodium storage with excellent electrochemical properties. The obtained composite possesses a cladding structure with homogeneous nanosheets as the outermost and CNT film as the inner network matrix, providing abundant ion diffusion channels, high electronic conductivity, and good mechanical flexibility. Due to these merits, this material possesses an excellent electrochemical performance for sodium storage, including a high specific capacity up to 390 mAh g-1 at 50 mA g-1, good rate performance up to 205 mAh g-1 at 500 mA g-1, and excellent cycling stability. On this basis, this work would bring a promising material for various energy storage devices and other emerging applications.

Laser direct writing derived robust carbon nitride films with efficient photon-to-electron conversion for multifunctional photoelectrical applications

Carbon nitride,an emerging polymeric semiconductor,has attracted attention in research ranging from photocatalysis to photodetection due to its favorable visible light response and high physicochemical stability.For its practical device application,the fabrication of high-quality carbon nitride films on substrates is essential.However,conventional methodologies to achieve high polymerization of carbon nitride are often accompanied by its decomposition,significantly compromising the film quality.Herein,we report an ultrafast fabrication of carbon nitride film by laser direct writing(LDW).The instantaneous high temperature and pressure during LDW can efficiently boost the polymerization of carbon nitride and suppress its decomposition,resulting in high-quality carbon nitride film with excellent mechanical stability with the substrate.Due to the efficient photon-to-electron conversion,it exhibits an outstanding photoelectrochemical water splitting and optoelectronic detection capability,even under strong acid/alkaline conditions.This study thus offers a facile and efficient LDW strategy for the rapid fabrication of carbon nitride film photoelectrodes,demonstrating its great feasibility in multifunctional photoelectrical applications,including but not limited to photoelectrochemical water splitting and optoelectronic detection.

Ion-exchange-induced Bi and K dual-doping of TiOx in molten salts for high-performance electrochemical nitrogen reduction

Electrocatalytic nitrogen reduction reaction (e NRR) at the ambient conditions is attractive for ammonia(NH_(3)) synthesis due to its energy-efficient and eco-friendly features. However, the extremely strong N≡N triple-bonds in nitrogen molecules and the competitive hydrogen evolution reaction lead to the unsatisfactory NH_(3) yield and the Faradaic efficiency (FE) of e NRR, making the development of high-performance catalysts with adequate active sites and high selectivity essential for further development of e NRR.Addressing this, we herein report a Bi and K dual-doped titanium oxide (BTO@KTO) material, which is prepared by a cation exchange reaction between K_(2)Ti_(4)O_(5) and molten BiCl_(2), for high-performance e NRR catalysts. Benefiting from the controllable molten-salt cation exchange process, a highly active surface containing Bi/K sites and rich oxygen vacancies has been obtained on titanium oxide. Under the synergy of these two merits, an efficient e NRR catalysis, with the NH_(3) yield rate of 32.02 μg h^(-1)mg_(cat)^(-1) and the FE of 12.71%, has been achieved, much superior to that of pristine K_(2)Ti_(4)O_(9). This work thus offers a highperformance electrocatalyst for e NRR, and more importantly, a versatile cation-exchange strategy for efficiently manipulating materials’ functionalities.

Extrusion-Based 3D-Printed Supercapacitors:Recent Progress and Challenges

Supercapacitors have been regarded as promising power supplies for future electronics due to their high power density,superior stability,easy integration,and safety.Extrusion-based three-dimensional printing technologies hold promise to satisfy the demands for integrated and flexible supercapacitors because of their highly versatile manufacturing process.In this review article,a comprehensive and timely review of these state-of-theart technologies is presented.We start with a brief introduction of fundamental concepts of supercapacitors,including energy storage mechanisms and device structures.Then,the latest progress of extrusionbased three-dimensional printing technologies(e.g.,fused deposition modeling,inkjet printing,and direct ink writing)along with their applications for manufacturing supercapacitors is summarized.The choice of printable materials(e.g.,graphene,carbon nanotubes,metal oxides,and MXenes),printing process,and the resulted electrochemical performances of supercapacitors are especially emphasized.Finally,the development of extrusion-based three-dimensional printing supercapacitors is summarized,with existing challenges diagnosed,possible solutions proposed,and future outlooks forecasted.We hope this review can offer insights to further improve the performance of three-dimensional-printed supercapacitors for practical applications.

Gastric pyloric gland adenoma resembling a submucosal tumor:A case report

BACKGROUND Pyloric gland adenoma(PGA)is a recently described and rare tumor.Submucosal tumor(SMT)-like PGA is more difficult to diagnose and differentiate from other submucosal lesions.CASE SUMMARY We present the case of a 69-year-old man with a 10 mm SMT-like elevated lesion with an opening in the upper part of the gastric body,referred to our hospital for further endoscopic treatment.Magnifying endoscopy with narrow-band imaging,endoscopic ultrasonography,and complete endoscopic submucosal dissection were performed on the patient.Histopathological findings revealed tightly packed tubular glands lined with cuboidal or columnar cells that had round-tooval nuclei containing occasional prominent nucleoli and an eosinophilic cytoplasm similar to that in non-neoplastic gastric pyloric glands.Additionally,immunohistochemical analysis showed positive staining for both mucin 5AC and mucin 6.Therefore,we arrived at the final diagnosis of gastric PGA.Although there was no apparent malignant component in this tumor,PGA has been considered a precancerous disease with a high risk of transformation into adenocarcinoma.CONCLUSION PGA should be considered when detecting gastric SMT-like lesions.Physicians and pathologists should focus on PGA due to its malignant potential.

Recent Progress of Conductive Metal-Organic Frameworks for Electrochemical Energy Storage

The development of reliable and low-cost energy storage systems is of considerable value in using renewable and clean energy sources,and exploring advanced electrodes with high reversible capacity,excellent rate performance,and long cycling life for Li/Na/Zn-ion batteries and supercapacitors is the key problem.Particularly because of their diverse structure,high specific surface area,and adjustable redox activity,electrically conductive metal-organic frameworks(c-MOFs)are considered promising candidates for these electrochemical applications,and a detailed overview of the recent progress of c-MOFs for electrochemical energy storage and their intrinsic energy storage mechanism helps realize a comprehensive and systematic understanding of this progress and further achieve highly efficient energy storage and conversion.Herein,the chemical structure of c-MOFs and their conductive mechanism are first introduced.Subsequently,a comprehensive summarization of the current applications of c-MOFs in energy storage systems,namely supercapacitors,LIBs,SIBs,and ZIBs,is presented.Finally,the prospects and challenges of c-MOFs toward much higher-performance energy storage devices are presented,which should illuminate the future scientific research and practical applications of c-MOFs in energy storage fields.

Promoting exciton dissociation by metal ion modification in polymeric carbon nitride for photocatalysis

Carbon nitride,a typical low-dimensional conjugated polymer photocatalyst,features a high exciton binding energy due to the weak dielectric screening and the strong Coulombic attraction of photogenerated electrons and holes.The reduction of the exciton binding energy of carbon nitride to promote the conversion from excitons into free carriers is the first priority for the improvement of charge-transfer-dependent photocatalytic reaction activity.In this paper,by introducing a variety of polar metal cations to carbon nitride,it is demonstrated that the charge distribution of the heptazine ring can be improved by ion polarization,which effectively promotes the dissociation of excitons into electrons and holes.The sodium ion shows the best modification effect,which enhances the rate of both photocatalytic hydrogen and hydrogen peroxide production by about 50%.Characterization shows that the introduction of strongly polar metal cations contributes to the reduction of the exciton dissociation energy of carbon nitride.This study provides a new perspective and a convenient method for the exciton modulation engineering of low-dimensional photocatalysts.

Partial anammox achieved in full scale biofilm process for typical domestic wastewater treatment

The slow initiation of anammox for treating typical domestic wastewater and the relatively high footprint of wastewater treatment infrastructures are major concerns for practical wastewater treatment systems.Herein,a 300 m^(3)/d hybrid biofilm reactor(HBR)process was developed and operated with a short hydraulic retention time(HRT)of 8 h.The analysis of the bacterial community demonstrated that anammox were enriched in the anoxic zone of the HBR process.The percentage abundance of Candidatus Brocadia in the total bacterial community of the anoxic zone increased from 0 at Day 1 to 0.33%at Day 130 and then to 2.89%at Day 213.Based upon the activity of anammox bacteria,the removal of ammonia nitrogen(NH_(4)^(+)-N)in the anoxic zone was approximately 15%.This showed that the nitrogen transformation pathway was enhanced in the HBR system through partial anammox process in the anoxic zone.The final effluent contained 12 mg/L chemical oxygen demand(COD),0.662 mg/L NH_(4)^(+)-N,7.2 mg/L total nitrogen(TN),and 6 mg/L SS,indicating the effectiveness of the HBR process for treating real domestic wastewater.

Mechanical Properties and Damage Tolerance of Bulk Yb_3Al_5O_(12) Ceramic

Yb3Al5O12has potential applications as thermal barrier coatings（TBCs） because it shows low thermal conductivity and close thermal expansion coefficient to nickel-based superalloys.As a prospective TBC material,besides superior thermal properties,the mechanical properties are also important.In this paper,we present the mechanical properties of Yb3Al5O12including elastic moduli,hardness,strength,and fracture toughness.The Young’s modulus of Yb3Al5O12is 282 GPa.The shear-modulus-to-bulkmodulus ratio of Yb3Al5O12is 0.63,which indicates relatively low shear deformation resistance.In addition,Yb3Al5O12exhibits high strength and fracture toughness but low hardness compared to yttria stabilized zirconia（YSZ）,the most successful TBC material.SEM observation reveals that the fracture surface of Yb3Al5O12displays 'layered structure feature',which is caused by crack deflection.Investigation based on Hertzian contact test demonstrates that Yb3Al5O12is a damage-tolerant ceramic.Crack deflection and bridging can arouse shear faults,dissipate the local damage energy,and restrict the crack propagation within the material,which play an important role in enhancing the damage tolerance.The superior mechanical properties and good damage tolerance ensure Yb3Al5O12a promising candidate for TBC applications.

New class of high-entropy pseudobrookite titanate with excellent thermal stability,low thermal expansion coefficient,and low thermal conductivity

As a type of titanate,the pseudobrookite(MTi_(2)O_(5)/M_(2)TiO_(5))exhibits a low thermal expansion coefficient and thermal conductivity,as well as excellent dielectric and solar spectrum absorption properties.However,the pseudobrookite is unstable and prone to decomposing below 1200℃,which limits the practical application of the pseudobrookite.In this paper,the high-entropy pseudobrookite ceramic is synthesized for the first time.The pure high-entropy(Mg,Co,Ni,Zn)Ti_(2)O_(5) with the pseudobrookite structure and the biphasic high-entropy ceramic composed of the highentropy pseudobrookite(Cr,Mn,Fe,Al,Ga)_(2)TiO_(5) and the high-entropy spinel(Cr,Mn,Fe,Al,Ga,Ti)_(3)O_(4) are successfully prepared by the in-situ solid-phase reaction method.The comparison between the theoretical crystal structure of the pseudobrookite and the aberration-corrected scanning transmission electron microscopy(AC-STEM)images of high-entropy(Mg,Co,Ni,Zn)Ti_(2)O_(5) shows that the metal ions(M and Ti ions)are disorderly distributed at the A site and the B site in high-entropy(Mg,Co,Ni,Zn)Ti_(2)O_(5),leading to an unprecedentedly high configurational entropy of high-entropy(Mg,Co,Ni,Zn)Ti_(2)O_(5).The bulk high-entropy(Mg,Co,Ni,Zn)Ti_(2)O_(5) ceramics exhibit a low thermal expansion coefficient of 6.35×10^(−6) K^(−1) in the temperature range of 25-1400℃ and thermal conductivity of 1.840 W·m^(−1)·K^(−1) at room temperature,as well as the excellent thermal stability at 200,600,and 1400℃.Owing to these outstanding properties,high-entropy(Mg,Co,Ni,Zn)Ti_(2)O_(5) is expected to be the promising candidate for high-temperature thermal insulation.This work has further extended the family of different crystal structures of high-entropy ceramics reported to date.

Electrocatalytic Oxygen Reduction to Produce Hydrogen Peroxide:Rational Design from Single‑Atom Catalysts to Devices

Electrocatalytic production of hydrogen peroxide(H_(2)O_(2))via the 2e^(-) transfer route of the oxygen reduction reaction(ORR)offers a promising alternative to the energy-intensive anthraquinone process,which dominates current industrial-scale production of H_(2)O_(2).The availability of cost-effective electrocatalysts exhibiting high activity,selectivity,and stability is imperative for the practical deployment of this process.Single-atom catalysts(SACs)featuring the characteristics of both homogeneous and heterogeneous catalysts are particularly well suited for H_(2)O_(2) synthesis and thus,have been intensively investigated in the last few years.Herein,we present an in-depth review of the current trends for designing SACs for H_(2)O_(2) production via the 2e^(-)ORR route.We start from the electronic and geometric structures of SACs.Then,strategies for regulating these isolated metal sites and their coordination environments are presented in detail,since these fundamentally determine electrocatalytic performance.Subsequently,correlations between electronic structures and electrocatalytic performance of the materials are discussed.Furthermore,the factors that potentially impact the performance of SACs in H_(2)O_(2)production are summarized.Finally,the challenges and opportunities for rational design of more targeted H_(2)O_(2)-producing SACs are highlighted.We hope this review will present the latest developments in this area and shed light on the design of advanced materials for electrochemical energy conversion.