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With the ever-increasing demands of grid-scale energy storage, aqueous zinc-ion batteries (ZIBs) have garnered increasing attention around the world. However, limited Zn2+ host materials have hindered the commercialization of ZIBs. Hence, Mo-V oxides with different phase structures (orth-, tri-, and tetra-MoVO) were precisely constructed to develop phase-dependent Mo-V oxide cathodes for Zn2+ storage in ZIBs. The open frameworks and varied tunnel structures formed a favorable alternative for achieving suitable Zn2+ diffusion kinetics. With optimized phase engineering, the high specific capacity of approximately 400 mA h g−1 and excellent cyclic stability of 1000 cycles were achieved with orth-MoVO as the cathode. The large amount of six- and seven-member rings in the orth-MoVO phase, which allow for alternative Zn2+ insertion, play a vital role in hosting Zn2+ ions reversibly. The proposed phase engineering strategy provides a new approach toward cathode design in ZIBs.

Ultrabroad spectral absorption is required for semiconductor photocatalysts utilized for solar-to-chemical energy conversion. The light response range can be extended by element doping, but the photocatalytic performance is generally not enhanced correspondingly. Here we present a solid alkali activation strategy to synthesize near-infrared (NIR) light-activated carbon-doped polymeric carbon nitride (A-cPCN) by combining the copolymerization of melamine and 1,3,5-trimesic acid. The prepared A-cPCN is highly crystalline with a narrowed bandgap and enhanced efficiency in the separation of photogenerated electrons and holes. Under irradiation with NIR light (780 nm ≥ λ ≥ 700 nm), A-cPCN shows an excellent photocatalytic activity for H2 generation from water with rate of 165 µmol g−1 h−1, and the photo-redox activity for H2O2 production (109 µmol g−1 h−1) from H2O and O2, whereas no observed photocatalytic activity over pure PCN. The NIR photocatalytic activity is due to carbon doping, which leads to the formation of an interband level, and the alkali activation that achieved shrinking the transfer distance of photocarriers. The current synergistic strategy may open insights to fabricate other carbon-nitrogen-based photocatalysts for enhanced solar energy capture and conversion.

Tandem water electrolysis for the transformation of universal feedstock to value-added chemicals integrated with hydrogen generation and in situ utilization is a promising approach to address the economic challenges of electrochemical hydrogen evolution and storage. Herein, we present the controllable electrocatalytic deuteration of halides using inexpensive and reusable heavy water (D2O) as a D-source for the preparation of valuable D-labelled chemicals and pharmaceuticals under mild conditions. This electrochemical deuteration method with high efficiency and selectivity furnishes a series of D-labelled chemicals and pharmaceuticals in high yields with excellent D-incorporation. The reaction efficiency and selectivity, that is, the precise substitution of deuterium atoms at different halogen positions, can be tuned by varying the applied voltages. The results show the great potential of green and economical electrocatalytic methods for producing value-added fine chemicals in addition to hydrogen evolution.

Zeolitic octahedral metal oxides (ZOMOs) are fully inorganic crystalline materials, mostly containing transition metals, and possess a defined framework as well as regular hollow channels. Therefore, they have significant application potential in many fields, particularly catalysis. Herein, we report the synthesis and characterization of zeolitic octahedral niobium oxides (ZOMO-NbOx) and the framework was made of {NbOx} polyhedra ({NbO6} octahedron and {Nb6O27} pentagon units). Microchannels consisting of 7-membered rings with ∼0.4 nm diameter were realized, and rarely reported plural {Nb6O27} units including dimers, trimers, and tetramers were discovered. Owing to the continuous hollow microporous structure that provides a large surface area as well as a shortened transfer path for charge carriers from bulk to the surface, considerably enhanced activities beyond pristine Nb2O5 were achieved towards photocatalytic H2 evolution from (saline) water. The results show a practical case of solo-Nb-based zeolitic materials, which expand the ZOMO family and provide further insights into the design and synthesis of efficient zeolitic semiconductors for artificial photocatalysis.

The development of cost-effective and high-performance catalysts for the production of hydrogen via electrocatalytic water splitting is crucial for meeting the increasing energy demand and expanding the hydrogen economy. In this study, a series of metal-free carbon nanotube (CNT) catalysts were designed and in situ functionalized by imidazolium ionic liquids (ILs) for enhanced electrocatalytic hydrogen evolution reaction (HER). The theoretical calculations and experimental results reveal that the functionalization of CNTs with imidazolium ILs facilitated the electron transfer process and exhibited superior hydrogen adsorption, thereby enhancing the performance of the HER. In particular, CNT-IM-Cl displays excellent electrocatalytic activity and shows a low onset overpotential and Tafel slope of 80 mV and 38 mV dec-1, respectively. This study highlights the significant potential of IL in situ functionalized metal-free CNTs for the electrocatalytic HER and provides insight into the structure design of highly efficient electrocatalysts.

Hydrogenation/deuteration of carbon chloride (C−Cl) bonds is of high significance but remains a remarkable challenge in synthetic chemistry, especially using safe and inexpensive hydrogen donors. In this article, a visible-light-photocatalytic watersplitting hydrogenation technology (WSHT) is proposed to in-situ generate active H-species (i.e., Had) for controllable hydrogenation of aryl chlorides instead of using flammable H2. When applying heavy water-splitting systems, we could selectively install deuterium at the C−Cl position of aryl chlorides under mild conditions for the sustainable synthesis of high-valued added deuterated chemicals. Sub-micrometer Pd nanosheets (Pd NSs) decorated crystallined polymeric carbon nitrides (CPCN) is developed as the bifunctional photocatalyst, whereas Pd NSs not only serve as a cocatalyst of CPCN to generate and stabilize H (D)-species but also play a significant role in the sequential activation and hydrogenation/deuteration of C−Cl bonds. This article highlights a photocatalytic-WSHT for controllable hydrogenation/deuteration of low-cost aryl chlorides, providing a promising way for the photosynthesis of high-valued added chemicals instead of the hydrogen evolution.

Booming of photocatalytic water splitting technology (PWST) opens a new avenue for the sustainable synthesis of high-value-added hydrogenated and oxidized fine chemicals, in which the design of efficient semiconductors for the in-situ and synergistic utilization of photogenerated redox centers are key roles. Herein, a porous polymeric carbon nitride (PPCN) with a crystalline backbone was constructed for visible light-induced photocatalytic hydrogen generation by photoexcited electrons, followed by in-situ utilization for olefin hydrogenation. Simultaneously, various alcohols were selectively transformed to valuable aldehydes or ketones by photoexcited holes. The porosity of PPCN provided it with a large surface area and a short transfer path for photogenerated carriers from the bulk to the surface, and the crystalline structure facilitated photogenerated charge transfer and separation, thus enhancing the overall photocatalytic performance. High reactivity and selectivity, good functionality tolerance, and broad reaction scope were achieved by this concerted photocatalysis system. The results contribute to the development of highly efficient semiconductor photocatalysts and synergistic redox reaction systems based on PWST for high-value-added fine chemical production.

Two-dimensional (2D) organic–inorganic hybrid perovskites (OIHPs) have recently drawn great interest due to their easy synthesis and excellent photoelectric properties. With tunable bandgaps, 2D OI...

A crystalline orthorhombic Mo–V–Cu oxide (MoVCuO) was successfully obtained by hydrothermal synthesis using a methylammonium cation as a structure-directing agent, and catalytic role of Cu for sele...

Zeolitic octahedral metal oxides (ZOMOs) are fully inorganic crystalline materials, mostly containing transition metals, and possess a defined framework as well as regular hollow channels. Therefore, they have significant application potential in many fields, particularly catalysis. Herein, we report the synthesis and characterization of zeolitic octahedral niobium oxides (ZOMO-NbOx) and the framework was made of {NbOx} polyhedra ({NbO6} octahedron and {Nb6O27} pentagon units). Microchannels consisting of 7-membered rings with ∼0.4 nm diameter were realized, and rarely reported plural {Nb6O27} units including dimers, trimers, and tetramers were discovered. Owing to the continuous hollow microporous structure that provides a large surface area as well as a shortened transfer path for charge carriers from bulk to the surface, considerably enhanced activities beyond pristine Nb2O5 were achieved towards photocatalytic H2 evolution from (saline) water. The results show a practical case of solo-Nb-based zeolitic materials, which expand the ZOMO family and provide further insights into the design and synthesis of efficient zeolitic semiconductors for artificial photocatalysis.

The development of cost-effective and high-performance catalysts for the production of hydrogen via electrocatalytic water splitting is crucial for meeting the increasing energy demand and expanding the hydrogen economy. In this study, a series of metal-free carbon nanotube (CNT) catalysts were designed and in situ functionalized by imidazolium ionic liquids (ILs) for enhanced electrocatalytic hydrogen evolution reaction (HER). The theoretical calculations and experimental results reveal that the functionalization of CNTs with imidazolium ILs facilitated the electron transfer process and exhibited superior hydrogen adsorption, thereby enhancing the performance of the HER. In particular, CNT-IM-Cl displays excellent electrocatalytic activity and shows a low onset overpotential and Tafel slope of 80 mV and 38 mV dec-1, respectively. This study highlights the significant potential of IL in situ functionalized metal-free CNTs for the electrocatalytic HER and provides insight into the structure design of highly efficient electrocatalysts.

With the ever-increasing demands of grid-scale energy storage, aqueous zinc-ion batteries (ZIBs) have garnered increasing attention around the world. However, limited Zn2+ host materials have hindered the commercialization of ZIBs. Hence, Mo-V oxides with different phase structures (orth-, tri-, and tetra-MoVO) were precisely constructed to develop phase-dependent Mo-V oxide cathodes for Zn2+ storage in ZIBs. The open frameworks and varied tunnel structures formed a favorable alternative for achieving suitable Zn2+ diffusion kinetics. With optimized phase engineering, a high specific capacity of approximately 400 mAh g−1 and the excellent cyclic stability of 1000 cycles were achieved with orth-MoVO as the cathode. The large amount of six- and seven-member rings in the orth-MoVO phase, which allow for alternative Zn2+ insertion, played a vital role in hosting Zn2+ ions reversibly. The proposed phase engineering strategy provides a new approach toward cathode design in ZIBs.

Photocatalytic water splitting technology (PWST) enables the direct use of water as appealing "liquid hydrogen source" for transfer hydrogenation reactions. Currently, the development of PWST-based transfer hydrogenations is still in an embryonic stage. Previous reports generally centered on the rational utilization of the in situ generated H-source (electrons) for hydrogenations, in which photogenerated holes were quenched by sacrificial reagents. Herein, the fully-utilization of the liquid H-source and holes during water splitting is presented for photo-reductive N -alkylation of nitro-aromatic compounds. In this integrate system, H-species in situ generated from water splitting were designed for nitroarenes reduction to produce amines, while alkanols were oxidized by holes for cascade alkylating of anilines as well as the generated secondary amines. More than 50 examples achieved with a broad range scope validate the universal applicability of this mild and sustainable coupling approach. The synthetic utility of this protocol was further demonstrated by the synthesis of existing pharmaceuticals via selective N -alkylation of amines. This strategy based on the sustainable water splitting technology highlights a significant and promising route for selective synthesis of valuable N -alkylated fine chemicals and pharmaceuticals from nitroarenes and amines with water and alkanols.

Precisely controlled deuterium labeling at specific sites of N-alkyl drugs is crucial in drug-development as over 50% of the top-selling drugs contain N-alkyl groups, in which it is very challenging to selectively replace protons with deuterium atoms. With the goal of achieving controllable isotope-labeling in N-alkylated amines, we herein rationally design photocatalytic water-splitting to furnish [H] or [D] and isotope alkanol-oxidation by photoexcited electron-hole pairs on a polymeric semiconductor. The controlled installation of N-CH3, -CDH2, -CD2H, -CD3, and -13CH3 groups into pharmaceutical amines thus has been demonstrated by tuning isotopic water and methanol. More than 50 examples with a wide range of functionalities are presented, demonstrating the universal applicability and mildness of this strategy. Gram-scale production has been realized, paving the way for the practical photosynthesis of pharmaceuticals., Controllable deuteration of N-alkyl amines is crucial in drug-development as they constitute over 50% of the top-selling drugs. Here, the authors report a polymeric semiconductor acting as photocatalyst in water-splitting and in isotope alkanol-oxidation by photoexcited electron-hole pairs, and furnishing deuterated amines.

Porous carbon nitride photocatalysts with sufficient cyanide groups were facile fabricated through simple calcination process with cheap salt as porogen. The introduction of cyanide groups can enhance charge separation efficiency and reductive activities of photogenerated electrons of carbon nitride. The optimized CN-S catalysts can selectively oxidize alcohols to aldehydes with broad scope as well as reduce oxygen to H2O2. The tandem strategy can photocatalytic produce H2O2 with a rate of more than 200 μmol h−1 g−1 which is nearly 19 times than that without alcohols and fulfilled utilization of both photo-generated electrons and holes.

Constructing heterojunction between two semiconductors is a cost-effective pathway to fabricate efficient photocatalysts for environmental remediation and energy-related applications, which is with profound significance and high desirability to contemporary era. In this work, we demonstrate an extremely facile approach to couple bismuth subcarbonate with polymeric carbon nitride (denoted as BIOC@PCN) by ion exchange between home-made rose-like Bi2O2(OH)(NO3) (denoted as BION) and PCN bulks at 433 K solvothermal condition. PCN bulks play multi-roles in this ingenious one-pot method. Firstly, PCN bulks guarantee the negatively charged surface to anchor plentiful bismuth precursor salts. More importantly, solvothermal treatment affords a weak basic and sufficient CO32− ions environment to promote the following ion exchange reaction. The evolution of morphology, components and structure from rose-like BION to BIOC@PCN were symmetrically characterized by means of SEM, HR-TEM, XRD, FTIR, TG, UV–vis, BET-BJH and XPS. The as-prepared nanohybrid photocatalyst (0.5BIOC@PCN) presents optimal photocatalytic performance for gaseous acetaldehyde removal, which is showing 10, 6.5 and 2 times higher than that of the PCN-Bulk, BION and mechanical mixed BIOC/PCN counterparts, respectively. Transient photocurrent response and EPR results further verify the validity of the established heterojunction of BIOC@PCN in facilitating the separation of charge carriers. The performance improvement gains from the efficient separation of charge carriers in BIOC@PCN heterojunction, manifested by PL spectra, transient photocurrent response and EPR results. In this study, a facile and cost-effective approach to build PCN-based nanohybrid photocatalysts for gaseous acetaldehyde efficient removal was established.

Developing economical and efficient electrocatalysts with nonprecious metals for the hydrogen evolution reaction (HER), especially in water-alkaline electrolyzers, is pivotal for large-scale hydrogen production. Recently, both density functional theory (DFT) calculations and experimental studies have demonstrated that earth-abundant MoS2 is a promising HER electrocatalyst in acidic solution. However, the HER kinetics of MoS2 in alkaline solution still suffer from a high overpotential (90–220 mV at a current density of 10 mA cm–2). Herein, we report a combined experimental and first-principle approach toward achieving an economical and ultraefficient MoS2-based electrocatalyst for the HER by fine-tuning the electronic structure of MoS2 nanorods with N and Mn dopants. The developed N,Mn codoped MoS2 catalyst exhibits an outstanding HER performance with overpotentials of 66 and 70 mV at 10 mA cm–2 in alkaline and phosphate-buffered saline media, respectively, and corresponding Tafel slopes of 50 and 65 mV de...

The development of graphene oxide (GO)-based materials for C-C cross-coupling represents a significant advance in carbocatalysis. Although GO has been used widely in various catalytic reactions, the scope of reactions reported is quite narrow, and the relationships between the type of functional groups present and the specific activity of the GO are not well understood. Herein, we explore CH-CH-type cross-coupling of xanthenes with arenes using GO as real carbocatalysts, and not as stoichiometric reactants. Mechanistic studies involving molecular analogues, as well as trapped intermediates, were carried out to probe the active sites, which were traced to quinone-type functionalities as well as the zigzag edges in GO materials. GO-catalyzed cross-dehydrogenative coupling is operationally simple, shows reusability over multiple cycles, can be conducted in air, and exhibits good functional group tolerance.

Solar-driven H2 evolution is an essential process for sustainable energy development. Currently, the greatest challenge is the development of efficient photocatalysts to drive this reaction, especially in pure water systems (without the use of a sacrificial agent). In this study, structural defects in Zn-Cd-S nanorod photocatalysts are found to increase charge separation efficiency significantly by sevenfold. Efficient H2 evolution (352.7 μmol h-1 g-1 , 100 mg of catalyst) is achieved by using this defective Zn-Cd-S nanorod photocatalyst in the absence of sacrificial agents and precious metal cocatalysts under visible-light irradiation. Thus, this cocatalyst- and sacrificial-agent-free, visible-light-responsive system shows remarkable potential as a new artificial photosynthesis route for green H2 production.

Crystalline Mo–V–W–O complex oxides with the orthorhombic or trigonal structure were synthesized by a hydrothermal method. Those Mo–V–W–O samples with various amounts of tungsten were characterized by inductively coupled plasma atomic emission spectroscopy, TEM, STEM–EDX, X-ray diffraction, Rietveld analysis, and a N2 adsorption method. It was found for the first case that an additional metal such as W can be successfully incorporated into the trigonal Mo–V–O structure by using (CH3CH2NH3)2Mo3O10.The alkylammonium cation acted as a structural stabilizer that was requisite for the formation of a trigonal structure when additional metal ions were present. For the orthorhombic Mo–V–W–O structure, introduction of W into the orthorhombic structure caused a rod segregation effect by which nanoscale crystals formed and the external surface area greatly increased. Additionally, these Mo–V–W–O materials were applied as catalysts for the gas phase selective oxidation of acrolein to acrylic acid. The best ca...

We succeeded in introducing W in Mo3VOx with keeping the orthorhombic, trigonal, and amorphous structures. Synthesized crystalline Mo(W)3VOx with orthorhombic and trigonal structures, both of which possess heptagonal channels, showed catalytic activity for gas-phase selective acrolein oxidation to acrylic acid superior to amorphous Mo(W)3VOx and to tetragonal Mo3VOx. The results strongly suggest that the crystalline Mo(W)3VOx with orthorhombic and trigonal structures are real active phase of industrial acrolein oxidation catalysts based on Mo, W, and V oxides. Furthermore, we found that the resulting W-containing catalyst showed less-dependency of water partial pressure in the reactant feed on the acrolein conversion.

Controllable deuteration of organic molecules to produce value‐added deuterium‐labelled chemicals and pharmaceutical compounds attracts growing interest in organic synthesis, tracer investigation and the pharmaceutical industry. In article number 1801403, Chenliang Su and co‐workers present a strategy based on water‐splitting‐technology for visible‐light photocatalytic selective deuteration of alkenes and alkynes over a highly crystalline and catalytically active K‐intercalated polymeric carbon nitride.

Crystalline Mo–V–W–O complex oxides with the orthorhombic or trigonal structure were synthesized by a hydrothermal method. Those Mo–V–W–O samples with various amounts of tungsten were characterized by inductively coupled plasma atomic emission spectroscopy, TEM, STEM–EDX, X-ray diffraction, Rietveld analysis, and a N2 adsorption method. It was found for the first case that an additional metal such as W can be successfully incorporated into the trigonal Mo–V–O structure by using (CH3CH2NH3)2Mo3O10.The alkylammonium cation acted as a structural stabilizer that was requisite for the formation of a trigonal structure when additional metal ions were present. For the orthorhombic Mo–V–W–O structure, introduction of W into the orthorhombic structure caused a rod segregation effect by which nanoscale crystals formed and the external surface area greatly increased. Additionally, these Mo–V–W–O materials were applied as catalysts for the gas phase selective oxidation of acrolein to acrylic acid. The best catalyst was assigned to the orthorhombic Mo–V–O–W7.5, which possessed an ordered arrangement of heptagonal and hexagonal channels and a large external surface area.

A series of WO 3 –ZrO 2 carriers were prepared by co-precipitation method with different mass fractions (0 wt%, 5 wt%, 10 wt%, 15 wt% and 20 wt%) of WO 3 , and MnO x –CeO 2 /WO 3 –ZrO 2 monolith catalysts were prepared for selective catalytic reduction of NO x with ammonia (NH 3 -SCR) in the presence of excessive O 2 . The catalysts were characterized by N 2 adsorption–desorption, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and NH 3 /NO temperature-programmed desorption (NH 3 /NO-TPD). The experimental results showed that, the tungsten modified monolith catalyst MnO x –CeO 2 /WO 3 –ZrO 2 with the WO 3 content 10 wt% had the best catalytic activity and the widest reaction window; it possessed a better thermal stability than V 2 O 5 /WO 3 /TiO 2 catalyst, and showed a better H 2 O and SO 2 tolerance than MnO x –CeO 2 /ZrO 2 . The characterization results indicated that MnO x –CeO 2 /10% WO 3 –ZrO 2 had the best textural properties, a well-dispersed state of WO 3 , the lowest binding energy of Ce 3+ 3d 5/2 , the maximum value of Ce 3+ :Ce=20.7%, the suitable molar ratio of Mn:Ce≈1, and a co-existence state of MnO 2 –Mn 2 O 3 . In addition, it had the most adsorbed sites of NH 3 or NO species. The NO x conversion was more than 80% in the temperature range of 150 °C to 380 °C at the space velocity of 10,000 h −1 . It possessed better potential for practical application.

A series of tungsten modified MnOx–CeO2 monolith catalysts were prepared and used for selective catalytic reduction (SCR) of NO by NH3 in the presence of O2. The experimental results showed that the SCR performance and SO2-resistant ability of MnOx–CeO2 were greatly enhanced by the introduction of tungsten. The catalyst containing 10% WO3 showed the highest NO conversion in a wide temperature range of 162–374 °C. The highly dispersed or amorphous tungsten oxide and the strong interaction between tungsten and MnOx–CeO2 should be the reasons for the excellent performance of the catalyst containing 10% WO3.

MnO x /CeO 2 –ZrO 2 –Al 2 O 3 (MnO x /CZA) catalysts with different amounts of manganese loading were prepared by incipient wetness impregnation method for selective catalytic reduction (SCR) of NO with NH 3 at low temperature. The catalysts were characterized by N 2 adsorption–desorption measurement, XRD, XPS, and H 2 -TPR. Catalytic activity tests reveal that the MnO x /CZA catalyst with 10% manganese loading has the best catalytic activity, almost 90% NO is translated to N 2 in the temperature range of 143–300 °C. The highly dispersed MnO x species, the good oxidation activity of NO to NO 2 , the existent synergistic effect between the manganese and cerium oxides, and the various oxidation states of manganese oxides may be the main reasons for the best SCR activity. In addition, the SCR activity is slightly influenced in the presence of SO 2 and H 2 O, while such effect is restorable after heating treatment.

In addition to the significance of photocatalytic hydrogen evolution, the utilization of the in situ generated H/D (deuterium) active species from water splitting for artificial photosynthesis of high value‐added chemicals is very attractive and promising. Herein, photocatalytic water splitting technology is utilized to generate D‐active species (i.e., Dad) that can be stabilized on anchored 2nd metal catalyst and are readily for tandem controllable deuterations of carbon–carbon multibonds to produce high value‐added D‐labeled chemicals/pharmaceuticals. A highly crystalline K cations intercalated polymeric carbon nitride (KPCN), rationally designed, and fabricated by a solid‐template induced growth, is served as an ultraefficient photocatalyst, which shows a greater than 18‐fold enhancement in the photocatalytic hydrogen evolution over the bulk PCN. The photocatalytic in situ generated D‐species by superior KPCN are utilized for selective deuteration of a variety of alkenes and alkynes by anchored 2nd catalyst, Pd nanoparticles, to produce the corresponding D‐labeled chemicals and pharmaceuticals with high yields and D‐incorporation. This work highlights the great potential of developing photocatalytic water splitting technology for artificial photosynthesis of value‐added chemicals instead of H2 evolution.

The development of highly active, inexpensive, and stable bifunctional oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalysts to replace noble metal Pt and RuO2 catalysts remains a considerable challenge for highly demanded reversible fuel cells and metal–air batteries. Here, a simple approach for the facile construction of a defective nanocarbon material is reported with B and N dopants (B,N‐carbon) as a superior bifunctional metal‐free catalyst for both ORR and OER. The catalyst is prepared by pyrolyzing the composites of ethyl cellulose and high‐boiling point 4‐(1‐naphthyl)benzeneboronic acid in NH3 atmosphere with an inexpensive Zn‐based template. The obtained porous B,N‐carbon with rich carbon defects exhibits excellent ORR and OER performances, including high activity and stability. In alkaline medium, B,N‐carbon material shows high ORR activity with an onset potential (E onset) reaching 0.98 V versus reversible hydrogen electrode (RHE), very close to that of Pt/C, a high electron transfer number and excellent stability. This catalyst also presents the admirable ORR activity in acidic medium with a high E onset of 0.81 V versus RHE and a four‐electron process. The OER activity of B,N‐carbon is superior to that of the precious metal RuO2 and Pt/C catalysts. A Zn–air battery using B,N‐carbon as the air cathode exhibits a low voltage gap between charge and discharge and long‐term stability. The excellent electrocatalytic performance of this porous nanocarbon material is attributed to the combined positive effects of the abundant carbon defects and the heteroatom codopants.