Development and Simulation of Sulfur‐doped Graphene Supported Platinum with Exemplary Stability and Activity Towards Oxygen Reduction

Sulfur‐doped graphene (SG) is prepared by a thermal shock/quench anneal process and investigated as a unique Pt nanoparticle support (Pt/SG) for the oxygen reduction reaction (ORR). Particularly, SG is found to induce highly favorable catalyst‐support interactions, resulting in excellent half‐cell based ORR activity of 139 mA mg_Pt ^?1 at 0.9 V vs RHE, significant improvements over commercial Pt/C (121 mA mg_Pt ^?1) and Pt‐graphene (Pt/G, 101 mA mg_Pt ^?1). Pt/SG also demonstrates unprecedented stability, maintaining 87% of its electrochemically active surface area following accelerated degradation testing. Furthermore, a majority of ORR activity is maintained, providing 108 mA mg_Pt ^?1, a remarkable 171% improvement over Pt/C (39.8 mA mg_Pt ^?1) and an 89% improvement over Pt/G (57.0 mA mg_Pt ^?1). Computational simulations highlight that the interactions between Pt and graphene are enhanced significantly by sulfur doping, leading to a tethering effect that can explain the outstanding electrochemical stability. Furthermore, sulfur dopants result in a downshift of the platinum d‐band center, explaining the excellent ORR activity and rendering SG as a new and highly promising class of catalyst supports for electrochemical energy technologies such as fuel cells.     

Structure Design Reveals the Role of Au for ORR Catalytic Performance Optimization in PtCo‐Based Catalysts

Au‐incorporation is a promising strategy to retard composition‐loss in Pt‐based catalyst. However, the unclear mechanism limits guided catalyst design and the performance optimization. Here, direct evidence is provided to validate the outward diffusion of Au atoms in Au‐core/Pt‐based‐shell structures. A Co interlayer is built between the Au‐core and PtCo‐based shell to exclude the possibility of atomic diffusion caused by interfacial alloying. In conjunction with the improved catalytic durability of the Au‐core@Pt‐based‐shell structure, it is reasonable to conclude that it is the subsurface segregated Au atoms rather than interfacial interaction that boosts the catalytic durability of Au‐core/Pt‐based‐shell structured catalysts towards oxygen reduction reaction. More importantly, by constructing Au‐core@Co‐interlayer@PtCoAu‐shell multilayer structure, the specific (1.730 mA cm^?2) and mass (0.692 A mg^?1_Pt) activities are enhanced 7‐ and 4‐ fold relative to the commercial Pt/C. After 10 000 cycles of accelerated durability test, the mass activity loss for the multilayered catalyst is as low as 6.14% while the loss exceeds 35% for the commercial Pt/C catalyst. The improved catalytic performance of the Au@Co@PtCoAu multilayer structure can be ascribed to the finely modulated electronic structure and the compensated composition loss owing to the delicate structure and composition profile design.     

Ultrasmall Pd‐Cu‐Pt Trimetallic Twin Icosahedrons Boost the Electrocatalytic Performance of Glycerol Oxidation at the Operating Temperature of Fuel Cells

Recently, in order to improve the energy conversion efficiency of direct polyol fuel cells, the engineering of effective Pd‐ and/or Pt‐based electrocatalysts to rupture C? C bonds has received increasing attention. Here, an example is shown to synthesize highly uniform sub‐10 nm Pd‐Cu‐Pt twin icosahedrons by controlling the nucleation phase. Because of the synergies of the electronic effect, synergistic effect, geometric effect, and abundant surface active sites originating from the formation of near surface alloy and special icosahedral shape, the Pd‐Cu‐Pt twin icosahedrons exhibit excellent electrocatalytic performance in glycerol electrocatalysis at the operating temperature of direct alcohol fuel cells (70 °C) in KOH electrolyte. The Pd_50.2Cu_38.4Pt_11.4 icosahedrons show mass activities of 9.7 A mg^?1_Pd+Pt and 13.7 A mg^?1_Pd. Furthermore, the Pd_50.2Cu_38.4Pt_11.4 icosahedrons demonstrate long‐term durability in current–time test for 36 000 s and high in situ anti‐CO poisoning performance. In addition, the introduction of CO can enhance electro‐oxidation endurance on Pd_50.2Cu_38.4Pt_11.4 icosahedrons, and the peak mass activity can reach to 14.4 A mg^?1_Pd+Pt. The in situ Fourier transform infrared spectroscopy spectra indicate that the Pd_50.2Cu_38.4Pt_11.4 icosahedrons possess a high capacity to break C? C bonds and may efficiently convert glycerol into CO₂, thus improving the utilization efficiency of energy‐containing molecule glycerol.     

The Quasi‐Pt‐Allotrope Catalyst: Hollow PtCo@single‐Atom Pt1 on Nitrogen‐Doped Carbon toward Superior Oxygen Reduction

Single‐atom Pt and bimetallic Pt₃Co are considered the most promising oxygen reduction reaction (ORR) catalysts, with a much lower price than pure Pt. The combination of single‐atom Pt and bimetallic Pt₃Co in a highly active nanomaterial, however, is challenging and vulnerable to agglomeration under realistic reaction conditions, leading to a rapid fall in the ORR. Here, a sustainable quasi‐Pt‐allotrope catalyst, composed of hollow Pt₃Co (H‐PtCo) alloy cores and N‐doped carbon anchoring single atom Pt shells (Pt₁N‐C), is constructed. This unique nanoarchitecture enables the inner and exterior spaces to be easily accessible, exposing an extra‐high active surface area and active sites for the penetration of both aqueous and organic electrolytes. Moreover, the novel Pt₁N‐C shells not only effectively protect the H‐PtCo cores from agglomeration but also increase the efficiency of the ORR in virtue of the isolated Pt atoms. Thus, the H‐PtCo@Pt₁N‐C catalyst exhibits stable ORR without any fade over a prolonged 10 000 cycle test at 0.9 V in HClO₄ solution. Furthermore, this material can offer efficient and stable ORR activities in various organic electrolytes, indicating its great potential for next‐generation lithium–air batteries as well.     

Very High Performance Alkali Anion‐Exchange Membrane Fuel Cells

Anion‐exchange membrane fuel cells (AEMFCs) have emerged as an alter‐native technology to overcome the technical and cost issues of proton‐exchange membrane fuel cells (PEMFCs). In this study, we describe a new electrocatalyst for AEMFCs composed of carbon nanotubes (CNTs), KOH‐doped polybenzimidazole (PBI) and platinum nanoparticles (Pt), in which the CNTs are wrapped by KOH‐doped PBI at a nanometer thickness and Pt is efficiently loaded on the wrapping layer. In the electrocatalyst, it is revealed that the CNTs and the KOH‐doped PBI layer function as electron‐ and hydroxide‐conductive paths, respectively, and the large exposed surface of the Pt allows an effective access of the fuel gas. Quantitative formation of the well‐defined interfacial structure formed by these components leads to an excellent mass transfer in the catalyst interface and realizes a high fuel‐cell performance. Membrane electrode assemblies fabricated with the electrocatalyst show a high power density of 256 mW cm^?2. To the best of our knowledge, this is the highest value for AEMFC systems measured in similar experimental conditions.     

Layer‐Controlled and Wafer‐Scale Synthesis of Uniform and High‐Quality Graphene Films on a Polycrystalline Nickel Catalyst

Chemical vapor deposition (CVD) provides a synthesis route for large‐area and high‐quality graphene films. However, layer‐controlled synthesis remains a great challenge on polycrystalline metallic films. Here, a facile and viable synthesis of layer‐controlled and high‐quality graphene films on wafer‐scale Ni surface by the sequentially separated steps of gas carburization, hydrogen exposure, and segregation is developed. The layer numbers of graphene films with large domain sizes are controlled precisely at ambient pressure by modulating the simplified CVD process conditions and hydrogen exposure. The hydrogen exposure assisted with a Ni catalyst plays a critical role in promoting the preferential segregation through removing the carbon layers on the Ni surface and reducing carbon content in the Ni. Excellent electrical and transparent conductive performance, with a room‐temperature mobility of ≈3000 cm² V^?1 s^?1 and a sheet resistance as low as ≈100 Ω per square at ≈90% transmittance, of the twisted few‐layer grapheme films grown on the Ni catalyst is demonstrated.     

Metal–Organic Framework-Derived N-Doped Carbon with Controllable Mesopore Sizes for Low-Pt Fuel Cells

Mesoporous structure of carbon materials plays an important role in electrocatalyst design. Constructing carbon supports with tunable mesopores has long been a challenge. Herein, the elaborate regulation of mesopores in N-doped carbon materials is reported by pyrolyzing energetic metal-triazolate (MET) frameworks with different particle sizes and at different ramp rates. Higher thermal transfer rates brought about by smaller particle size and higher ramp rate lead to more violent decomposition with a large number of gases producing, which in turn result in larger mesopores in the derivatives. Consequently, a series of N-doped carbon materials with controllable mesopores are obtained. As a proof-of-concept, ultrafine Pt nanoparticles are enveloped inside these mesopores to acquire high-performance electrocatalysts for oxygen reduction reaction. The optimized catalyst achieves high mass activity of 1.52 A mg_Pt⁻¹ at 0.9 V_iR-free and peak power density of 0.8 W cm⁻² (H₂-Air) with an ultralow Pt loading of 0.05 mg_Pt cm⁻² at cathode in fuel cells, highlighting the great advantages of MET-derived carbon materials with controllable mesopores in the preparation of advanced electrocatalysts.     

Phase and Composition Tuning of 1D Platinum‐Nickel Nanostructures for Highly Efficient Electrocatalysis

Among various platinum (Pt)‐based nanostructures, porous or hollow ones are of great importance because they exhibit fantastic oxygen reduction reaction (ORR) enhancements and maximize atomic utilization by exposing both exterior and interior surfaces. Here, a new class of porous Pt₃Ni nanowires (NWs) with 1D architecture, an ultrathin Pt‐rich shell, high index facets, and a highly open structure is designed via a selective etching strategy by using the phase and composition segregated Pt‐Ni NWs as the starting material. The porous feature of Pt₃Ni NWs can be readily fulfilled by changing the Pt/Ni atomic ratio of the starting Pt‐Ni NWs. Such porous Pt₃Ni NWs show extraordinary activity and stability enhancements toward methanol oxidation reaction and ORR. The porous Pt₃Ni NWs can deliver ORR mass activity of 5.60 A mg^?1, which is 37.3‐fold higher than that of the Pt/C. They also show outstanding stability with negligible activity loss after 20 000 cycles. This study offers a unique approach for the design of complex nanostructures as efficient catalysts through precisely tailoring.     

Electrically Conductive Thin Films Prepared from Layer‐by‐Layer Assembly of Graphite Platelets

Layer‐by‐layer (LBL) assembly of carbon nanoparticles for low electrical contact resistance thin film applications is demonstrated. The nanoparticles consist of irregularly shaped graphite platelets, with acrylamide/ββ‐methacryl‐oxyethyl‐trimethyl‐ammonium copolymer as the cationic binder. Nanoparticle zeta (ζζ) potential and thereby electrostatic interactions are varied by altering the pH of graphite suspension as well as that of the binder suspension. Film thickness as a function of zeta potential, immersion time, and the number of layers deposited is obtained using Monte Carlo simulation of the energy dispersive spectroscopy measurements. Multilayer film surface morphology is visualized via field‐emission scanning electron microscopy and atomic‐force microscopy. Thin film electrical properties are characterized using electrical contact resistance measurements. Graphite nanoparticles are found to self‐assemble onto gold substrates through two distinct yet overlapping mechanisms. The first mechanism is characterized by logarithmic carbon uptake with respect to the number of deposition cycles and slow clustering of nanoparticles on the gold surface. The second mechanism results from more rapid LBL nanoparticle assembly and is characterized by linear weight uptake with respect to the number of deposition cycles and a constant bilayer thickness of 15 to 21 nm. Thin‐film electrical contact resistance is found to be proportional to the thickness after equilibration of the bilayer structure. Measured values range from 1.6 mΩ cm^?2 at 173 nm to 3.5 mΩ cm^?2 at 276 nm. Coating volume resistivity is reduced when electrostatic interactions are enhanced during LBL assembly.     

Heteroatom (N or N‐S)‐Doping Induced Layered and Honeycomb Microstructures of Porous Carbons for CO2 Capture and Energy Applications

Increasing global challenges such as climate change, environmental pollution, and energy shortage have stimulated the worldwide explorations into novel and clean materials for their applications in the capture of carbon dioxide, a major greenhouse gas, and toxic pollutants, energy conversion, and storage. In this study, two microstructured carbons, namely N‐doped pillaring layered carbon (NC) and N, S codoped honeycomb carbon (NSC), have been fabricated through a one‐pot pyrolysis process of a mixture containing glucose, sodium bicarbonate, and urea or thiourea. The heteroatom doping is found to induce tailored microstructures featuring highly interconnected pore frameworks, high sp²‐C ratios, and high surface areas. The formation mechanism of the varying pore frameworks is believed to be hydrogen‐bond interactions. NSC displays a similar CO₂ adsorption capacity (4.7 mmol g^?1 at 0 °C), a better CO₂/N₂ selectivity, and higher activity in oxygen reduction reaction as compared with NC‐3 (the NC sample with the highest N content of 7.3%). NSC favors an efficient four‐electron reduction pathway and presents better methanol tolerance than Pt/C in alkaline media. The porous carbons also exhibit excellent rate performance as supercapacitors.     

Replicating the Defect Structures on Ultrathin Rh Nanowires with Pt to Achieve Superior Electrocatalytic Activity toward Ethanol Oxidation

Metal nanostructures with an ultrathin Pt skin and abundant surface defects are attractive for electrocatalytic applications owing to the increased utilization efficiency of Pt atoms and the presence of highly reactive sites. This paper reports a conformal, layer‐by‐layer deposition of Pt atoms on defective Rh nanowires for the faithful replication of surface defects (i.e., grain boundaries) on the Rh nanowires. The thickness of the Pt shell can be controlled from one monolayer up to 5.3 atomic layers. This series of Rh@Pt_nL (n = 1–5.3) core–sheath nanowires show greatly enhanced activity and durability in catalyzing the ethanol oxidation reaction in an acidic medium. Among others, the Rh @ Pt_3.5L nanowires show the greatest mass activity (809 mA mg^?1_Pt) and specific activity (1.18 mA cm^?2) after loaded on carbon support, which are 3.7 and 3.4 times those of the commercial Pt/C, respectively. In situ Fourier transform infrared spectroscopy studies indicate an enhanced interaction between the outermost Pt layer and the Rh nanowire can promote C? C bond cleavage for complete oxidation of ethanol to CO₂ while depress the dehydrogenation of ethanol to acetic acid. As the Pt shell thickness is increased, the selectivity for the CO₂ pathway decreases while that for acetic acid is increased.     

Few‐Layer MoSe2 Nanosheets with Expanded (002) Planes Confined in Hollow Carbon Nanospheres for Ultrahigh‐Performance Na‐Ion Batteries

Sodium‐ion batteries (SIBs) are considered as a promising alternative to lithium‐ion batteries, due to the abundant reserves and low price of Na sources. To date, the development of anode materials for SIBs is still confronted with many serious problems. In this work, encapsulation‐type structured MoSe₂@hollow carbon nanosphere (HCNS) materials assembled with expanded (002) planes few‐layer MoSe₂ nanosheets confined in HCNS are successfully synthesized through a facile strategy. Notably, the interlayer spacing of the (002) planes is expanded to 1.02 nm, which is larger than the intrinsic value of pristine MoSe₂ (0.64 nm). Furthermore, the few‐layer nanosheets are space‐confined in the inner cavity of the HCNS, forming hybrid MoSe₂@HCNS structures. When evaluated as anode materials for SIBs, it shows excellent rate capabilities, ultralong cycling life with exceptional Coulombic efficiency even at high current density, maintaining 501 and 471 mA h g^?1 over 1000 cycles at 1 and 3 A g^?1, respectively. Even when cycled at current densities as high as 10 A g^?1, a capacity retention of 382 mA h g^?1 can be achieved. The expanded (002) planes, 2D few‐layer nanosheets, and unique carbon shell structure are responsible for the ultralong cycling and high rate performance.     

Fe,Cu‐Coordinated ZIF‐Derived Carbon Framework for Efficient Oxygen Reduction Reaction and Zinc–Air Batteries

Zeolitic imidazole frameworks (ZIFs) offer rich platforms for rational design and construction of high‐performance nonprecious‐metal oxygen reduction reaction (ORR) catalysts owing to their flexibility, hierarchical porous structures, and high surface area. Herein, an Fe, Cu‐coordinated ZIF‐derived carbon framework (Cu@Fe‐N‐C) with a well‐defined morphology of truncated rhombic dodecahedron is facilely prepared by introducing Fe²⁺ and Cu²⁺ during the growth of ZIF‐8, followed by pyrolysis. The obtained Cu@Fe‐N‐C, with bimetallic active sites, large surface area, high nitrogen doping level, and conductive carbon frameworks, exhibits excellent ORR performance. It displays 50 mV higher half‐wave potential (0.892 V) than that of Pt catalysts in an alkaline medium and comparable performance to Pt catalysts in an acidic medium. In addition, it also has excellent durability and methanol resistance ability in both acidic and alkaline solutions, which makes it one of the best Pt‐free catalysts reported to date for ORR. Impressively, when being employed as a cathode catalyst in zinc–air batteries, Cu@Fe‐N‐C presents a higher peak power density of 92 mW cm^?2 than that of Pt/C (74 mW cm^?2) as well as excellent durability.     

RhMoS2 Nanocomposite Catalysts with Pt‐Like Activity for Hydrogen Evolution Reaction

High overpotentials and low efficiency are two main factors that restrict the practical application for MoS₂, the most promising candidate for hydrogen evolution catalysis. Here, Rh?MoS₂ nanocomposites, the addition of a small amount of Rh (5.2 wt%), exhibit the superior electrochemical hydrogen evolution performance with low overpotentials, small Tafel slope (24 mV dec^?1), and long term of stability. Experimental results reveal that 5.2 wt% Rh?MoS₂ nanocomposite, even exceeding the commercial 20 wt% Pt/C when the potential is less than ?0.18 V, exhibits an excellent mass activity of 13.87 A mg_metal^?1 at ?0.25 V, four times as large as that of the commercial 20 wt% Pt/C catalyst. The hydrogen yield of 5.2 wt% Rh?MoS₂ nanocomposite is 26.3% larger than that of the commercial 20 wt% Pt/C at the potential of ?0.25 V. The dramatically improved electrocatalytic performance of Rh?MoS₂ nanocomposites may be attributed to the hydrogen spillover from Rh to MoS₂.     

Selective Determination of Dopamine on a Boron‐Doped Diamond Electrode Modified with Gold Nanoparticle/Polyelectrolyte‐coated Polystyrene Colloids

Negatively charged gold nanoparticles (AuNPs) and a polyelectrolyte (PE) have been assembled alternately on a polystyrene (PS) colloid by a layer‐by‐layer (LBL) self‐assembly technique to form three‐dimensional (Au/PAH)₄/(PSS/PAH)₄ multilayer‐coated PS spheres (Au/PE/PS multilayer spheres). The Au/PE/PS multilayer spheres have been used to modify a boron‐doped diamond (BDD) electrode. Cyclic voltammetry is utilized to investigate the properties of the modified electrode in a 1.0 M KCl solution that contains 5.0 × 10^?3 M K₃Fe(CN)₆, and the result shows a dramatically decreased redox activity compared with the bare BDD electrode. The electrochemical behaviors of dopamine (DA) and ascorbic acid (AA) on the bare and modified BDD electrode are studied. The cyclic voltammetric studies indicate that the negatively charged, three‐dimensional Au/PE/PS multilayer sphere‐modified electrodes show high electrocatalytic activity and promote the oxidation of DA, whereas they inhibit the electrochemical reaction of AA, and can effectively be used to determine DA in the presence of AA with good selectivity. The detection limit of DA is 0.8 × 10^?6 M in a linear range from 5 × 10^?6 to 100 × 10^?6 M in the presence of 1 × 10^?3 M AA.     

Trimetallic Mn‐Fe‐Ni Oxide Nanoparticles Supported on Multi‐Walled Carbon Nanotubes as High‐Performance Bifunctional ORR/OER Electrocatalyst in Alkaline Media

Discovering precious metal‐free electrocatalysts exhibiting high activity and stability toward both the oxygen reduction (ORR) and the oxygen evolution (OER) reactions remains one of the main challenges for the development of reversible oxygen electrodes in rechargeable metal–air batteries and reversible electrolyzer/fuel cell systems. Herein, a highly active OER catalyst, Fe_0.3Ni_0.7O_X supported on oxygen‐functionalized multi‐walled carbon nanotubes, is substantially activated into a bifunctional ORR/OER catalyst by means of additional incorporation of MnO_X. The carbon nanotube‐supported trimetallic (Mn‐Ni‐Fe) oxide catalyst achieves remarkably low ORR and OER overpotentials with a low reversible ORR/OER overvoltage of only 0.73 V, as well as selective reduction of O₂ predominantly to OH^?. It is shown by means of rotating disk electrode and rotating ring disk electrode voltammetry that the combination of earth‐abundant transition metal oxides leads to strong synergistic interactions modulating catalytic activity. The applicability of the prepared catalyst for reversible ORR/OER electrocatalysis is evaluated by means of a four‐electrode configuration cell assembly comprising an integrated two‐layer bifunctional ORR/OER electrode system with the individual layers dedicated for the ORR and the OER to prevent deactivation of the ORR activity as commonly observed in single‐layer bifunctional ORR/OER electrodes after OER polarization.     

Nitrogen‐Doped Nanoporous Carbon/Graphene Nano‐Sandwiches: Synthesis and Application for Efficient Oxygen Reduction

A zeolitic‐imidazolate‐framework (ZIF) nanocrystal layer‐protected carbonization route is developed to prepare N‐doped nanoporous carbon/graphene nano‐sandwiches. The ZIF/graphene oxide/ZIF sandwich‐like structure with ultrasmall ZIF nanocrystals (i.e., ≈20 nm) fully covering the graphene oxide (GO) is prepared via a homogenous nucleation followed by a uniform deposition and confined growth process. The uniform coating of ZIF nanocrystals on the GO layer can effectively inhibit the agglomeration of GO during high‐temperature treatment (800 °C). After carbonization and acid etching, N‐doped nanoporous carbon/graphene nanosheets are formed, with a high specific surface area (1170 m² g^?1). These N‐doped nanoporous carbon/graphene nanosheets are used as the nonprecious metal electrocatalysts for oxygen reduction and exhibit a high onset potential (0.92 V vs reversible hydrogen electrode; RHE) and a large limiting current density (5.2 mA cm^?2 at 0.60 V). To further increase the oxygen reduction performance, nanoporous Co‐N_x/carbon nanosheets are also prepared by using cobalt nitrate and zinc nitrate as cometal sources, which reveal higher onset potential (0.96 V) than both commercial Pt/C (0.94 V) and N‐doped nanoporous carbon/graphene nanosheets. Such nanoporous Co‐N_x/carbon nanosheets also exhibit good performance such as high activity, stability, and methanol tolerance in acidic media.     

Facile Synthesis of Manganese‐Oxide‐Containing Mesoporous Nitrogen‐Doped Carbon for Efficient Oxygen Reduction

Developing low‐cost non‐precious metal catalysts for high‐performance oxygen reduction reaction (ORR) is highly desirable. Here a facile, in situ template synthesis of a MnO‐containing mesoporous nitrogen‐doped carbon (m‐N‐C) nanocomposite and its high electrocatalytic activity for a four‐electron ORR in alkaline solution are reported. The synthesis of the MnO‐m‐N‐C nanocomposite involves one‐pot hydrothermal synthesis of Mn₃O₄@polyaniline core/shell nanoparticles from a mixture containing aniline, Mn(NO₃)₂, and KMnO₄, followed by heat treatment to produce N‐doped ultrathin graphitic carbon coated MnO hybrids and partial acid leaching of MnO. The as‐prepared MnO‐m‐N‐C composite catalyst exhibits high electrocatalytic activity and dominant four‐electron oxygen reduction pathway in 0.1 M KOH aqueous solution due to the synergetic effect between MnO and m‐N‐C. The pristine MnO shows little electrocatalytic activity and m‐N‐C alone exhibits a dominant two‐electron process for ORR. The MnO‐m‐N‐C composite catalyst also exhibits superior stability and methanol tolerance to a commercial Pt/C catalyst, making the composite a promising cathode catalyst for alkaline methanol fuel cell applications. The synergetic effect between MnO and N‐doped carbon described provides a new route to design advanced catalysts for energy conversion.     

Highly Efficient Electrocatalysts for Oxygen Reduction Reaction Based on 1D Ternary Doped Porous Carbons Derived from Carbon Nanotube Directed Conjugated Microporous Polymers

One‐dimensional (1D) porous materials have shown great potential for gas storage and separation, sensing, energy storage, and conversion. However, the controlled approach for preparation of 1D porous materials, especially porous organic materials, still remains a great challenge due to the poor dispersibility and solution processability of the porous materials. Here, carbon nanotube (CNT) templated 1D conjugated microporous polymers (CMPs) are prepared using a layer‐by‐layer method. As‐prepared CMPs possess high specific surface areas of up to 623 m² g^?1 and exhibit strong electronic interactions between p‐type CMPs and n‐type CNTs. The CMPs are used as precursors to produce heteroatom‐doped 1D porous carbons through direct pyrolysis. As‐produced ternary heteroatom‐doped (B/N/S) 1D porous carbons possess high specific surface areas of up to 750 m² g^?1, hierarchical porous structures, and excellent electrochemical‐catalytic performance for oxygen reduction reaction. Both of the diffusion‐limited current density (4.4 mA cm^?2) and electron transfer number (n = 3.8) for three‐layered 1D porous carbons are superior to those for random 1D porous carbon. These results demonstrate that layered and core–shell type 1D CMPs and related heteroatom‐doped 1D porous carbons can be rationally designed and controlled prepared for high performance energy‐related applications.     

A High‐Potential Anion‐Insertion Carbon Cathode for Aqueous Zinc Dual‐Ion Battery

Aqueous dual‐ion batteries (DIBs) are promising for large‐scale energy storage due to low cost and inherent safety. However, DIBs are limited by low capacity and poor cycling of cathode materials and the challenge of electrolyte decomposition. In this study, a new cathode material of nitrogen‐doped microcrystalline graphene‐like carbon is investigated in a water‐in‐salt electrolyte of 30 m ZnCl₂, where this carbon cathode stores anions reversibly via both electrical double layer adsorption and ion insertion. The (de)insertion of anions in carbon lattice delivers a high‐potential plateau at 1.85 V versus Zn²⁺/Zn, contributing nearly 1/3 of the capacity of 134 mAh g^?1 and half of the stored energy. This study shows that both the unique carbon structure and concentrated ZnCl₂ electrolyte play critical roles in allowing anion storage in carbon cathode for this aqueous DIB.