Heteroatom-doped Carbon Materials Research Articles

(Invited) Surface Electrochemistry and Physicochemical Behaviors of Carbon and Compound Electrodes in Electrochemical Separation Systems

In recent years, electrochemical separation systems have received a great attention due to their excellent capabilities in environmental remediation, water desalination, and resource recovery. The performances of electrochemical separation systems are often interpreted in terms of capacity and selectivity, both of which are highly dependent on electrode materials. For instance, capacitive deionization (CDI) used for desalination of water employs activated carbon electrodes, as it enables capture and release of sodium chloride in large amounts. In addition, lithium-ion selective electrode such as delithiated LiMn2O4 (i.e. λ-MnO2) or LiFePO4 plays an essential role in selectivity of electrochemical lithium recovery systems. However, although the importance electrode materials cannot be overemphasized for such electrochemical separations, it is also true that we are yet to achieve a sufficient level of understanding on their behaviors in the systems, which is necessary to establish rational electrode-design strategies to enhance capacity and selectivity of the electrochemical separation systems. In this talk, our recent findings on surface electrochemistry of carbon electrodes in electrochemical desalination will be introduced, together with an overview on the non-favorable Faradaic reactions thoroughly characterized with the assistance of various X-ray and electrochemical techniques. Additionally, development of heteroatom-doped carbon material and how it resulted in a highly stable CDI performance will be presented. Moreover, I will talk about our efforts on characterization of physicochemical behavior of λ-MnO2 in electrochemical lithium recovery systems, based on which a significantly higher utilization rate of the electrode materials could be achieved.

The extended Stӧber method for synthesizing nitrogen-doped porous carbon nanospheres supported Pt nanoparticles towards methanol oxidation in alkaline media

• N -doped porous carbon nanospheres were prepared via the extended Stӧber method. • The NPCs have a high surface area and abundant nitrogen content. • The Pt nanoparticles supported on NPCs showed superior MOR activity and stability. Heteroatom-doped porous carbon materials have emerged as attractive catalyst supports of Pt nanoparticles in the direct methanol fuel cells (DMFCs). Herein, the simple extended Stӧber method towards nitrogen-doped porous carbon nanospheres (NPCs) is reported by polymerizing of 3-aminophenol-formaldehyde (APF) resin spheres. The synthesized NPCs were applied as a carrier for Pt nanoparticles to fabricate the Pt@NPCs catalyst for methanol oxidation. Compared with the commercial Pt/C catalyst, Pt@NPCs showed the larger electrochemically active area (93.6 m 2 g −1 ), higher peak current density (95.91 mA·cm −2 ) and better stability in alkaline media. This improved performance can be attributed to the porous structure of NPCs and nitrogen atoms doped in the carbon matrix increasing the dispersion of the Pt particles on the NPCs catalyst.

Carbon doped with binary heteroatoms (N,X–C, where X = P, B, or S) derived from polypyrrole for enhanced electromagnetic wave absorption at microwave frequencies

Dual heteroatom-doped carbon materials show great promise as electromagnetic wave absorbers. However, synthesizing carbons containing multiple heteroatoms at controlled heteroatom doping levels has provided challenges to date. Herein, we report a simple method for manufacturing dual heteroatom doped carbons (N,X–C, where X = P, B, or S) by direct carbonization of polypyrrole synthesized in the presence of H3PO4, H3BO3, or H2SO4, respectively. The heteroatom content of the N,X–C products could be precisely tuned by varying amounts of acid dopant used in the polypyrrole synthesis. The N,X–C materials showed excellent electromagnetic wave absorption properties, especially N,S1–C (prepared using equimolar amounts of pyrrole and H2SO4) which offered a wide absorption bandwidth up to 6.6 GHz (11.38–18 GHz), and a RLmin of −32.3 dB (14.2 GHz) at 2.5 mm at a filler loading of 9.0 wt%. The outstanding electromagnetic wave absorption performance of N,S1–C was attributed to the presence of N dopant species, defects, C–S, and C–SOx groups, which optimized dipole polarization and conduction loss in the dielectric loss leading to excellent impedance matching.

Adsorption and catalysis of peroxymonosulfate on carbocatalysts for phenol degradation: The role of pyrrolic-nitrogen

Persulfate-based nonradical oxidation processes are appealing for removing refractory aromatic organic contaminants in wastewater purification. Here, ultrathin nitrogen-doped carbonaceous catalysts with different pyrrolic-N contents were developed by a facile modifiable g-C3N4-templated strategy. We observed that N-C-6 has the highest pyrrolic-N content, and the presence of N-C-6 with Peroxymonosulfate (PMS) achieved almost 98 % degradation for phenol degradation within 30 min. Moreover, the decisive role of pyrrolic-N in activating PMS was illustrated through experiments, instrument characterization and theoretical calculations: the more pyrrolic-N-doping could exhibit the higher redox potential of the metastable complex with PMS, and the stronger interaction between both materials, the greater PMS adsorption, as a result, the oxidation rate of phenol is faster by charge abstraction reactions. The results provide a new strategy for the intrinsic roles of heteroatom doped carbon materials to activate persulfates.

Design of aminated heteroatom-doped carbon materials with improved adsorption performance to uranium(VI)

Design of aminated heteroatom-doped carbon materials with improved adsorption performance to uranium(VI)

Fe-NX-C material with excellent supercapacitor performance prepared through oleic acid acidification pretreatment—Oily sludge pyrolysis process

Heteroatom-doped carbon materials derived from oil-bearing sludge exhibit excellent supercapacitor performance due to their unique electronic and chemical properties. However, the complex composition of heteroatoms in oil-bearing sludge makes it difficult to achieve sufficient and directional doping by direct pyrolysis. In this paper, an oleic acid pretreatment-roasting-secondary activation strategy was developed to make full use of hydrocarbons, iron- and nitrogen-containing compounds in oil-bearing sludge to prepare Fe-NX-C materials with excellent electrochemical properties. Characterization results such as transmission electron microscopy (TEM) and N2 adsorption analysis showed that the best sample had a hierarchical pore structure and uniform Fe and N element loading. X-ray photoelectron spectroscopy (XPS) analysis found that the addition of oleic acid can promote the formation of Fe-Nx, and the dosage of oleic acid will affect the content of Fe-Nx in the carbon materials. Electrochemical characterization of this supercapacitor material was conducted. The best sample's specific capacitance was as high as 293.6 F g−1 at the current density of 0.5 A g−1, and the capacitance retention rate could still reach 71.5% at the current density of 10 A g−1. The assembled button-type symmetrical supercapacitors had an energy density of 8.68 Wh kg−1 and a power density of 137.53 W kg−1, which is much higher than those of most other waste-based carbon materials. This work presents a new idea for the preparation of heteroatom doped carbon materials with excellent capacitive properties from oily sludge, which provides a new reference for the treatment and resource utilization of oily sludge.

Sacrificial Template-Assisted Mechanochemical Production of Highly Active Bifunctional Fe-N-C Catalysts

Bifunctional catalyst materials development for energy storage and conversion technologies is notoriously demanding in terms of electrochemistry (low stability, sluggish kinetics and high total overpotential (∆E)) and logistics (environmental safety, production methodologies and cost).Noble metal electrocatalysts are proven to be good bifunctional catalysts and as a result are being used as benchmark catalysts. However, the environmental and economic sustainability is severely compromised due to the scarcity of these metals. The alternative option is based on first-row transition metal heteroatom-doped carbon materials. Low cost, high availability, great electrocatalytic activity and stability promise to be a suitable noble metal free catalyst for oxygen evolution reaction (OER) and oxygen reduction reaction (ORR).This work showcases a high performance Fe-N-C type material with sustainable synthesis and efficient activity towards ORR and OER. Unlike various classical methods for electrocatalyst synthesis, the developed methodology combines mechanochemistry and application of sacrificial template, which yields materials with superior bifunctional oxygen electrocatalytic performance.

N, P dual doped foamy-like carbons with abundant defect sites for zinc ion hybrid capacitors

To achieve high value-added use of biomass waste is still a big challenge. Besides, heteroatom-doped carbon materials have been charmed enormous interests due to their high conductivity and abundant defect sites. Herein, a simply and confined pyrolysis method is innovated to prepare N, P codoped foamy-like carbons (NPFC) with abundant defect sites from osmanthus flowers. The NPFC features uniform N, P doped, porous structures and big electric conductivity, which provide abundant defects and additional active sites for ion adsorption, shorten ion transfer distance, enhance transfer kinetics and supply highways for electron transfer. As cathode for zinc ion hybrid capacitor (ZHC), NPFC exhibits large energy density (85.7 Wh kg−1) with long cycle life (remains 97.4% after 20,000 cycles) in aqueous electrolyte. More interestingly, NPFC-based quasi-solid-state ZHC presents extremely big capacity of 163.6 mAh g−1 at 0.1 A g−1 and excellent power density of 35.9 kW kg−1. This study offers a universal method to synthesize heteroatom-doped carbon materials from biomass waste for hybrid capacitors.

Poly(ionic liquid) Nanovesicle-Templated Carbon Nanocapsules Functionalized with Uniform Iron Nitride Nanoparticles as Catalytic Sulfur Host for Li-S Batteries.

Poly(ionic liquid)s (PIL) are common precursors for heteroatom-doped carbon materials. Despite a relatively higher carbonization yield, the PIL-to-carbon conversion process faces challenges in preserving morphological and structural motifs on the nanoscale. Assisted by a thin polydopamine coating route and ion exchange, imidazolium-based PIL nanovesicles were successfully applied in morphology-maintaining carbonization to prepare carbon composite nanocapsules. Extending this strategy further to their composites, we demonstrate the synthesis of carbon composite nanocapsules functionalized with iron nitride nanoparticles of an ultrafine, uniform size of 3–5 nm (termed “FexN@C”). Due to its unique nanostructure, the sulfur-loaded FexN@C electrode was tested to efficiently mitigate the notorious shuttle effect of lithium polysulfides (LiPSs) in Li–S batteries. The cavity of the carbon nanocapsules was spotted to better the loading content of sulfur. The well-dispersed iron nitride nanoparticles effectively catalyze the conversion of LiPSs to Li2S, owing to their high electronic conductivity and strong binding power to LiPSs. Benefiting from this well-crafted composite nanostructure, the constructed FexN@C/S cathode demonstrated a fairly high discharge capacity of 1085 mAh g–1 at 0.5 C initially, and a remaining value of 930 mAh g–1 after 200 cycles. In addition, it exhibits an excellent rate capability with a high initial discharge capacity of 889.8 mAh g–1 at 2 C. This facile PIL-to-nanocarbon synthetic approach is applicable for the exquisite design of complex hybrid carbon nanostructures with potential use in electrochemical energy storage and conversion.

Metal–organic framework-derived Co@NMPC as efficient electrocatalyst for hydrogen evolution reaction: Revealing the synergic effect of pyridinic N–Co

Developing hydrogen economy is one of the feasible routes to reduce carbon emission in response to the energy crisis and global warming. The hydrogen generation by electrochemical water splitting has received widespread attention, but it is still challenging to fabricate high-efficient electrocatalysts to decrease the kinetic energy barrier of hydrogen evolution reaction (HER). Loading transition metal (TM) nanoparticles (NPs) into heteroatom-doped carbon materials (HCM) has been reported as a capable scheme to increase the electrochemical activity and stability, but the synergic effect between TM surface and HCM is still worth exploring. Ascertaining that, we used metal-organic frameworks (MOFs) as the sacrificial precursor to synthesis a series of Co NPs encapsulated in N-doped microporous carbon (NMPC) nanocatalysts (denoted as Co@NMPC) with different N species (such as pyrrolic, pyridinic and graphitic N). The nanocatalyst prepared at an appropriate condition displayed an outstanding HER activity with an overpotential of 193 mV in 1 M KOH solution and 132 mV in 0.5 M H2SO4 solution to reach 10 mA cm−2 current density. Furthermore, the results of in situ shielding tests indicate that the synergy of pyridinic N–Co site owing to the intimate contact between Co surface and NMPC play the pivotal role in boosting HER performance. Density functional theory (DFT) calculations were employed to obtain an in-depth mechanism of synergic effect between Co and NMPC.

HNO3 pre-oxidation-tuned microstructures of porous carbon derived from high-sulfur coal for enhancing capture and catalytic conversion of polysulfides

Heteroatoms-doped carbon materials have received increasing interest as promising sulfur hosts for lithium-sulfur (Li-S) batteries. Herein, high-sulfur coal was selected as the low cost and earth-abundant precursor and HNO3 pre-oxidation was adopted to tune the microstructure of N,O,S-multidoped three-dimensional porous carbon (NOSTPC) to facilitate affinity and conversion toward polysulfides. HNO3 pretreatment significantly increases the specific surface area, pore volume, and the content of pyrrolic nitrogen and the defects in NOSTPCs. HNO3 pre-oxidation increases the specific capacity of Li-S battery with NOSTPC as the sulfur host from 559.3 to 860.4 mAh g−1 at 1C, and the capacity retention from 67% to 81% after 200 cycles. The satisfying performance benefits from that oxidation pretreatment improves the chemical adsorption of polysulfides by NOSTPC(O), and accelerates the kinetic conversion of polysulfides together with the catalytic oxidation of Li2S. Accordingly, the good performance of high-sulfur coal-based NOSTPCs can not only promote practical application of Li-S batteries, but also facilitate the efficient utilization of high-sulfur coal.

O- and F-doped porous carbon bifunctional catalyst derived from polyvinylidene fluoride for sulfamerazine removal in the metal-free electro-Fenton process

Heteroatom-doped carbon materials can effectively activate H2O2 into •OH during the metal-free electro-Fenton (EF) process. However, information on bifunctional catalysts for the simultaneous generation and activation of H2O2 is scarce. In this study, O- and F-doped porous carbon cathode materials (PPCs) were prepared by the direct carbonization of polyvinylidene fluoride (PVDF) for sulfamerazine (SMR) removal in a metal-free EF process. The porous structure and chemical composition of the PPCs were regulated by the carbonization temperature. PPC-6 (carbonized at 600 °C) exhibited optimal electrocatalytic performance in terms of electrochemical H2O2 generation and activation owing to its high specific surface area, mesoporous structure, and optimum fractions of doped O and F. Excellent performance of the 2e− oxygen reduction reaction was found with an H2O2 selectivity of 93.5% and an average electron transfer number of 2.13. An H2O2 accumulative concentration of 103.9 mg/L and an SMR removal efficiency of 90.1% were achieved during the metal-free EF process. PPC-6 was able to stably remove SMR over five consecutive cycles, retaining 92.6% of its original performance. Quantitative structure-activity relationship analysis revealed that doped oxygen functional groups contributed substantially to H2O2 generation, and semi-ionic C–F bonds with high electronegativity were the cause of the activation of H2O2 to •OH. These findings suggest that the PVDF-derived carbonaceous catalysts are feasible and desirable for metal-free EF processes.

Synthesis of coal tar pitch-derived heteroatom-doped porous carbon materials for aqueous zinc-ion hybrid supercapacitors

Zinc-ion hybrid supercapacitors (ZHSs), which combine the superiority of batteries and supercapacitors, will become a new development direction in the field of energy storage. The development of ZHSs with high capacity and high stability can be further promoted by heteroatom doping or structural modification of cathode materials. Herein, N,O,P co-doped porous carbon materials were synthesized by a facile method using coal tar pitch as precursor, aluminum phosphate as template, and sodium hydroxide as activator. Due to the high specific surface area and abundant micropores, the heteroatom-doped porous carbon materials were employed as cathode for aqueous ZHSs to study the electrochemical performance. Benefitted from the rich micropores and heteroatom doping, the porous carbon electrodes exhibit an outstanding electrochemical performance and deliver a large specific capacitance of 113.3 mA h g−1 at 0.1 A g−1. In addition, the porous carbon electrode shows a high energy density of 64.9 Wh kg−1 and a high power density of 1.23 kW kg−1, which outperforms most aqueous ZHS energy storage systems previously reported. Interestingly, after 5000 cycles at 1 A g−1, the specific capacity is about 36% higher than the original capacity and the coulomb efficiency still remains nearly 100%. The article may provide a new insight into exploring cathode materials for high-performance aqueous rechargeable zinc-ion energy storage devices.

Highly efficient adsorption of chromium on N, S-codoped porous carbon materials derived from paper sludge

The synergistic effect of heteroatoms is a viable method to enhance the adsorption performance of heavy metal onto carbon-based materials. However, the high cost, complex operation and a lot of pollution from the synthesis process have limited its development. Herein, a facile two-step pyrolysis method is used to prepare in situ N and S doped porous biochar from paper mill sludge for the removal of Cr(VI) from aqueous environment. The NSC-450 sample prepared under the optimum conditions has a large specific surface area of 3336.7 m2 g−1, an average pore size of 2.56 nm and a total pore volume of 2.10 cm3 g−1, manifesting the excellent adsorption capacity of 356.25 mg g−1 for Cr(VI). The adsorption of Cr(VI) by NSC-450 is consistent with the Langmuir isotherm and pseudo-second-order model, suggesting a spontaneous and endothermic chemisorption process. The analysis results show that the NH, graphitic nitrogen and thiophene structures have a positive effect on converting a large amount of Cr(VI) to Cr(III) by synergistic reduction, indicating obviously facilitating Cr(VI) removal compared to other sites. Therefore, in this material, the strong adsorption mechanism is mainly reductive complexation. Moreover, the effects of real water quality, anions, cations and fulvic acid on the adsorption behavior of Cr(VI) onto the NSC-450 were further investigated. The results demonstrate that the chromium removal rate remains above 82% even in actual electroplating wastewater, suggesting NSC-450 has great practical application prospect. This work offered a feasible method for high-value utilization of sludge, but also provided a novel perspective for the future design of heteroatom-doped carbon materials for promoting to eliminate hexavalent chromium from water environment.

Ru on N‐doped Carbon for the Selective Hydrogenolysis of Sugars and Sugar Alcohols

AbstractGlycols are accessible via metal‐catalyzed hydrogenolysis of sugar alcohols such as xylitol obtained from hemicellulose. Ru‐based catalysts are highly active but also catalyze side‐reactions such as decarbonylation and deoxygenation. To achieve high selectivity, these reactions need to be suppressed. In our study, we introduce heteroatom doped carbon materials as catalyst supports providing high selectivity. Heteroatom doping with nitrogen and oxygen was achieved by treating activated carbon with HNO3, NH3 and H2 or carbonization of organic precursors. For all N‐doped materials a high glycol selectivity of 80 % for sorbitol and xylitol and 44 % for xylose and glucose was reached. XPS analysis confirms the presence of different nitrogen species at the carbon surface and varying ligand effects for oxygen and nitrogen. Oxygen has an electron withdrawing effect on ruthenium and leads to a decreased activity. Nitrogen has weaker electron withdrawing properties, resulting in an enhanced selectivity.

Multi-heteroatom-doped hollow carbon nanocages from ZIF-8@CTP nanocomposites as high-performance anodes for sodium-ion batteries

Carbon-based material is one of the most promising candidates of anode materials for sodium-ion batteries (SIBs). However, the poor rate performance and low capacity due to intrinsic nature greatly impact their practical application. Heteroatom-doped carbon material is an efficient method to optimize the electrochemical performance of anode electrodes for SIBs. Herein, we report a template-initiated strategy to fabricate nitrogen, phosphorus, fluorine co-doped hollow carbon nanocages (NPF–HCN) derived from a rationally designed zeolitic imidazolate framework-8@covalent triazine polymer core-shell structured nanocomposites (ZIF-8@CTP). High proportions of tailored multi-heteroatom species within the CTP network contribute to the in-situ generation of N, P, F-doping in the resultant hollow carbon nanocages. Additionally, the hierarchical porous and hollow nanostructures of the NPF-HCN can promote the penetration of electrolytes, thus reduce diffusion barrier of Na+. As anode materials of SIBs, the as-prepared NPF-HCN delivers a higher initial capacity of 569.6 mA h/g at 1 A/g and a superior cycling behavior with a high capacity of 220.3 mA h/g at 5 A/g after 5000 cycles.

Waste Eggshell-derived N, P, S Tri-doped Core-shell Catalysts for Efficient Fenton-like Catalysis

Heteroatom-doped carbon materials have been proved as potent catalysts for the remediation of organic contaminants. Herein, molten salt electrolysis (MSE) was employed to convert waste eggshell and Co3O4 into N, P, S tri-doped core–shell catalyst (Co@NPSC), achieving the conversion of waste eggshell into value-added materials. Impressively, Co@NPSC/peroxymonosulfate (PMS) system exhibited an exceptional ultra-high turnover frequency (TOF) value of 83.86 min−1 for sulfamethoxazole (SMX) degradation with a low catalyst dosage of 0.001 g L–1. Subsequently, density functional theory (DFT) simulation clarified the synergistic essences of catalytic oxidation (i.e., the Co@NPSC catalyst reduced the adsorption energy of PMS molecular on its surface, reduced itself work function, enhanced the length of the O-O bond (IO-O) of PMS molecule, and facilitated electron transfer for PMS activation). In addition, both theoretical predictions and acute toxicity assay results indicated that the degradation of SMX equals detoxification. This work provides a new insight into the reutilization of waste eggshell and the design of heteroatom-doped core–shell catalysts.

Sustainable synthesis of heteroatom-doped porous carbon skeleton from Acacia auriculiformis bark for high-performance symmetric supercapacitor device

In recent years, the applications of biomass-derived meso/microporous carbon materials have fascinated increasing research attention due to their cost-effective and easy synthesis pathways. Researchers are using different types of biological precursors such as bark, leaves, roots, peels, fruits, and biological waste, etc., to synthesize porous carbon materials. In energy storage applications, the biomass-derived activated porous carbon may achieve an excellent capacitance, durability, and rate capability, compared to artificial nanomaterials, such as carbon nanotubes, fullerene, graphene, etc., due to their intrinsic and hierarchical structure. A clear understanding of the elemental and chemical composition, and porous nature of the biological precursor may be required to obtain a high-carbon yield, graphitized, high-energy, and power density carbon materials. In this work, novel heteroatom doped, and interconnected nanoflake-like porous carbon materials have been synthesized from Acacia auriculiformis bark for high-performance energy-density storage applications. The existence of the heteroatom in the carbon framework enhances the pseudocapacitive property of the materials. The synthesized porous carbon demonstrates the maximum specific capacitance 324 F g−1 and 288 F g−1 at 1 A g−1 current-density in acidic and neutral electrolytes, respectively. The electrokinetic analysis of the synthesized porous carbon materials demonstrates the maximum capacitive contribution to overall charge storage using both electrolytes. The fabricated solid-state symmetric device has a maximum capacitance of 107 F g−1 along with an energy density of 59.44 Wh kg−1 and power density of 10 kW kg−1. The synthesized heteroatom-doped porous carbon (H-PC) materials display outstanding durability up to 10,000 continuous cycles using a solid-state device even in strongly acidic conditions.

Pyrolyzing soft template-containing poly(ionic liquid) into hierarchical N-doped porous carbon for electroreduction of carbon dioxide

• Soft template-containing poly(ionic liquid) was pyrolyzed to N-doped carbon. • Porosity and N species were modulated by controlling pyrolysis temperatures. • The resultant carbon featured hierarchically small-/ultra-microporous structure. • High-proportioned surface Grap-N species served as the major active sites. • Hierarchical small-/ultra-micropores accounted for the electrocatalysis activity. Heteroatom-doped carbon materials have demonstrated great potential in the electrochemical reduction reaction of CO 2 (CO 2 RR) due to their versatile structure and function. However, rational structure control remains one challenge. In this work, we reported a unique carbon precursor of soft template-containing porous poly(ionic liquid) (PIL) that was directly synthesized via free-radical self-polymerization of ionic liquid monomer in a soft template route. Variation of the carbonization temperature in a direct pyrolysis process without any additive yielded a series of carbon materials with facile adjustable textural properties and N species. Significantly, the integration of soft-template in the PIL precursor led to the formation of hierarchical porous carbon material with a higher surface area and larger pore size than that from the template-free precursor. In CO 2 RR to CO, the champion catalyst gave a Faraday efficiency of 83.0% and a current density of 1.79 mA∙cm −2 at −0.9 V vs. reversible hydrogen electrode ( vs. RHE). The abundant graphite N species and hierarchical pore structure, especially the unique hierarchical small-/ultra-micropores were revealed to enable better CO 2 RR performance.

Three birds with one stone approach to superior N/S co-doped microporous carbon for gas storage and water purification

• N/S-co-doped microporous carbon (N/S-MPC) was synthesized by “three birds with one stone” activator, KSCN. • KSCN can also cooperate with K 2 CO 3 to improve the property of N/S-MPC material. • N/S-MPC material exhibited a superior methane storage performance (0.15 g/g). • N/S-MPC material can remove both organic pollutants and Pb 2+ with high capacity. Biomass-derived heteroatom-doped porous carbon materials play an indispensable role in energy storage and environment remediation. Currently, combined activation of porogen and organic dopant is resource consuming and complex. Here, a “three birds with one stone” activator, KSCN, was introduced to realize pore formation and N/S co-doping of porous carbon initiated by an oxygen displacement reaction. Multifunctional KSCN resulted in N/S-co-doped microporous carbon (N/S-MPC) materials with a high surface area (1906 m 2 /g, microporosity ≥ 82%) and N/S content. Most importantly, KSCN can also cooperate with K 2 CO 3 via a carbothermal reduction reaction to improve the surface area of N/S-MPC material to 2659 m 2 /g. Accordingly, both high microporosity and N/S co-doping of the resulting material led to superior methane storage performance (0.15 g/g) at 25 °C and 35 bar. These advantages also ensure that as-prepared material has unprecedented water purification capability for simultaneous organic pollutant and heavy metal (Pb 2+ ) removal by multiple mechanisms (pore-fitting, π–π bond, and complexation). This multifunctional activator provides a new direction for the design of high-performance biomass-derived carbon materials.