JOURNAL OF POWER SOURCES
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2026
·
IF 8.4
Shah Noor,Xiaoshuai Yu,Chunlin Li,Lei Sun,Zibo Zhao,Yan Liu,Chun Cheng Yang,Guoyong Wang
The rational design of high-performance electrocatalysts is essential for promoting the industrialization of electrocatalytic water-splitting technology. Herein, nitrogen-defects (Nd)-enriched g-C 3 N 4 (CN)-supported cobalt single-atom catalysts (Co-Nd/CN) are fabricated as high-efficiency bifunctional electrocatalysts for water splitting. Abundant Nd improves substrate conductivity and modulates the electronic structure of Co-N x active sites simultaneously. Benefiting from abundant coordination sites, lower charge transfer dynamics, and surface reactions, the optimized Co-Nd/CN exhibits the lowest overpotentials of 172 and 310 mV vs. RHE for HER and OER, respectively, at 10 mA cm −2 . Additionally, Co-Nd/CN delivers a full-cell voltage of 1.53 V at 10 mA cm −2 for overall water splitting with a Faradaic efficiency of 87.5%. Extended durability measurements demonstrate robust catalytic stability for Co-Nd/CN over 100 h of continuous operation. This work puts forward a novel approach based on elemental doping and defect engineering for the design of effective and enduring catalysts for water splitting.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Yunping Wu,Shuwen Niu,Zhengyu Wei,Lingzhe Meng,Wei Wei
Single-atom catalysts (SACs) with nitrogen-coordinated transition metal sites (M-N x ) hold great promise for electrocatalytic oxygen reduction and oxygen evolution reactions (ORR, OER). Despite substantial achievements based on the confinement pyrolysis and heteroatom-doping methods, the M-N x SACs still suffer from low yield of atomic sites and less tenability of electronic states of M-N x center. Here, an innovate synthesis methodology is proposed for surface integrating Co atoms onto polyoxometalate (POM) and its derivative clusters, which promise to regulate the atomic distribution and coordination environments of Co-N x SACs at the sub-nanometer level. The synthetic procedures exhibit general applicability for a variety of POM clusters to achieve high atomic Co loading up to 9.9 wt%. Steric integration by POM-derived clusters (e.g. MoN) also impart strengthened d-p orbital hybridization of Co-N x SACs by the formation of Co-N-Mo bonding, which surpass common heteroatoms toward modulating the geometric and electronic structures of M-N x SACs, leading to pronounced catalytic activity and durability. This work validates the effectiveness of the unique POM-integration strategy toward atomic dispersion of transition metal, further guides the engineering of M-N x SACs to promote catalytic performance from the sub-nanometer scale.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yi Wu,Junliang Chen,Jie Liu,Linjie Zhang,Reza Abazari,Ting-Ting Li,Jinjie Qian
The energy crisis heightens interest in proton exchange membrane fuel cells (PEMFCs), where the oxygen reduction reaction (ORR) is a critical cathodic process hindered by its intrinsic sluggish kinetics. Single-atom catalysts (SACs) at the molecular level, notably those featuring an Fe-N 4 structure derived from iron phthalocyanine (FePc), exhibit significant potential but confront the challenges of aggregation and inadequate electrical conductivity. Herein, we present a novel FePc coupled with defect-rich CoN x -doped hollow carbon nanostraw derived from cobalt-doped indium-based metal–organic frameworks (MOFs). This enhancement is attributed to the CoN x structure’s effective modulation of the Fe-N 4 active sites, further complemented by the hollow nanostraw structure, which significantly increases the accessibility of active sites, thereby promoting enhanced catalytic performance. FePc@HCoNC demonstrates exceptional ORR performance with an oxygen reduction potential of 0.903 V, half-wave potential of 0.914 V, and limiting current density of 5.18 mA cm −2 . For zinc-air batteries (ZABs), FePc@HCoNC achieves an open-circuit voltage of 1.524 V, peak power density of 153.06 mW cm −2 , specific capacity of 758.10 mAh g −1 , and stable cycling for 150 h. These findings underscore its potential as a superior alternative to precious metal-based catalysts, offering a pathway to more sustainable and efficient energy conversion technologies.
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Advanced Science
·
2025
·
IF 14.1
Lili Liu,Chen Wang,Luxin Zhao,Yayun Xiao,Weiwei Fang,Lanling Zhao,Faxing Wang,Yuping Wu
The practical development of Li-O 2 batteries (LOBs) urgently needs to explore robust cathode catalysts to boost the sluggish Li 2 O 2 reaction kinetics and parasitic reactions despite their theoretically high specific energy. Profound understanding of the cathode properties and the battery performance is rather critical in developing rational-designed electrocatalysts. In this study, a Co-N x /Co (111) decorated N-doped hierarchical carbon framework (Co-N x /Co@NHCF) is proposed as an efficient cathode in LOBs. Spectroscopic analysis coupled with experimental results suggests that the Co-N x /Co (111) catalytic center can significantly reduce the battery overpotential, and meanwhile, the hierarchical carbon framework ensures rapid mass transportation and provides sufficient space to accommodate Li 2 O 2 deposition. Density functional theory calculations reveal that the incorporated Co (111) facet can effectively regulate the electronic distribution of N-carbon, optimize the adsorption of desirable intermediates, and eventually facilitate oxygen reduction reaction/oxygen evolution reaction kinetics. As expected, the Co-N x /Co@NHCF catalyzed LOBs deliver a high discharge/charge capacity of 6.15/ 6.22 mAh cm −2 with a columbic efficiency of 98.9%, along with a high rate cycling of 700 h at 0.3 mA cm −2 . This work provides valuable instruction for the rational design of efficient catalysts for high-performance LOBs via optimization of the crystal structure and the adsorption of intermediates.
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JOURNAL OF POWER SOURCES
·
2021
·
IF 9.127
Xiangsi Wu,Chunlei Tan,Caimei He,Tong Zhao,Xianwen Wu,Zhaoling Ma,Hongqiang Wang,Yezheng Cai,Qiang Wu,Qingyu Li
Electrocatalyst is the pivotal component promoting the kinetics of oxygen reduction reaction in aqueous metal-air batteries . However, the content of increased bond as the active species is usually limited by the metal loading, tiny pore canal, insufficient nitrogen further restraining the electrocatalytic effectiveness of single-atom catalysts in oxygen reduction reaction (ORR). Herein, Co, N-dual doped carbon (Co/NNC) is prepared by a versatile strategy of the combination approach of SiO 2 template with extra nitrogen source. Based on ZIF-67 prepared with the assistance of SiO 2 template, the extra nitrogen source was introduced in the high-temperature pyrolysis procedure. The material characterizations of XRD , SEM, HRTEM , BET, Raman and XPS are conducted to synthetically analyze the functional role of extra nitrogen source. Moreover, the Co/NNC with increased Co-N x active sites is employed into two aqueous metal-air batteries of Zn-air and Mg-air batteries, which exhibits excellent performances especially in the aspects of discharge specific capacity, discharge stability and power density.
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ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Sun Lina,Sun Liping,Huo Lihua,Zhao Hui
The production of hydrogen peroxide (H 2 O 2 ) through electrochemically reducing O 2 in a two-electron pathway is a potential substitute for the traditional process based on anthraquinone. In this paper, F doping is carried out to prepare N and F co-doped porous carbon embedded Co nanoparticles. The electro-catalytic activity for the electrochemical production of H 2 O 2 is systematically investigated. The composite material demonstrates exceptional electro-catalytic selectivity, reaching approximately 92.5%, and shows an ultra-high rate of producing H 2 O 2 in 4021.4 mmol g -1 h -1 at 0.1 V versus RHE in a 0.5 M H 2 SO 4 electrolyte. It is found that the synergetic effect of Co-Nx and F in the composite material result in its exceptional performance. Adding F atom modulates the Zeta potential of the catalyst and alters the electronic configuration around Co-Nx, creating favorable conditions for the uptake of O 2 and consequently forming OOH*. Additionally, the highly electronegative F atom facilitate desorbing OOH* through electrostatic repulsion, preventing any further degradation. In a homemade electrolyzer containing 80 mg L -1 of Rh B, the H 2 O 2 produced in situ in a 0.5 M H 2 SO 4 electrolyte degrades up to 97.76% of Rh B in just 22.5 min, showcasing its potential for practical wastewater treatment applications.
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ADVANCED MATERIALS
·
2019
·Vol. 31
·期 11
·1808341
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IF 25.809
Wanbing Gong,Yue Lin,Chun Chen,Mohammad Al-Mamun,Hai-Sheng Lu,Guozhong Wang,Haimin Zhang,Huijun Zhao
Biomass is the most abundant renewable resource on earth and developing high-performance nonprecious selective hydrogenation (SH) catalysts will enable the use of biomass to replace rapidly diminishing fossil resources. This work utilizes ZIF-67-derived nitrogen-doped carbon nanotubes to confine Co nanoparticles (NPs) with Co–N x active sites as a high-performance SH catalyst. The confined Co NPs with Co–N x exhibit excellent catalytic activity, selectivity, and stability toward a wide range of biomass-derived compounds. Such active sites can selectively hydrogenate aldehyde, ketone, carboxyl, and nitro groups of biomass-derived compounds into value-added fine chemicals with 100% selectivity. The reported approach could be adopted to create other forms of catalytically active sites from other nonprecious metals.
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Reaction Chemistry & Engineering
·
2020
·Vol. 6
·期 1
·112-118
·
IF 3.441
Renjie Huang,Yanxin Wang,XiXi Liu,Peng Zhou,Shiwei Jin,Zehui Zhang
The selective hydrogenation of nitro compounds into their corresponding azo compounds is challenging in organic synthesis. In this study, we have developed a facile and efficient catalytic system for the transformation of nitro compounds into azo compounds under mild conditions over a heterogeneous cobalt catalyst (Co–Nx/C-800-AT). The Co–Nx/C-800-AT catalyst was found to be highly active for the reductive-coupling of nitro compounds into azo compounds in ethanol at 110 °C and 2.5 bar H2 pressure with the addition of NaOH as an additive, affording structurally-diverse azo compounds with satisfactory yields (70.4–98.3%). The developed method demonstrated several advantages such as high catalytic activity and high selectivity with tolerance to other functional groups and high stability.
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APPLIED SURFACE SCIENCE
·
2025
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IF 6.9
Qingwen Zheng,Zhuo Ma,Yunfeng Qiu,Zheng Zhang,Ruiwen Wang,Shaoqin Liu
Enhancing the performance of microbial fuel cells (MFCs) for sustainable energy generation requires innovative anode designs that facilitate efficient extracellular electron transfer (EET). This study presents a biomimetic approach to anode fabrication, developing a hierarchical Co-N x doped carbon nanotube/reduced graphene oxide (ZnCo/rGO@CC) composite inspired by the EET mechanisms of c-type cytochromes. The composite leverages the synergistic effects of Co-N x active sites, mimicking heme groups, and a three-dimensional porous structure to promote bacterial colonization and electron transfer. MFCs equipped with the ZnCo/rGO@CC anode achieved a maximum power density of 3.27 W/m 2 and a startup time of 1.68 days, significantly outperforming traditional carbon cloth anodes (1.49 W/m 2 and 2.50 days, respectively). Further demonstrating its potential for sustainable waste valorization, the MFC system was successfully operated using sugarcane bagasse as a fuel source, exhibiting a power density of 1.58 W/m 2 . Electrochemical analyses and microbial community characterization confirmed enhanced EET kinetics, selective enrichment of Geobacter (79.73 %), and robust biofilm formation on the ZnCo/rGO@CC anode. This biomimetic anode design, coupled with the utilization of sugarcane bagasse, offers a promising strategy for developing sustainable and efficient bioelectrochemical systems for cleaner energy production.
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JOURNAL OF POWER SOURCES
·
2021
·
IF 9.127
Li Zhong,Qi Huang,Junyang Ding,Yuanyuan Guo,Xian Wang,Lulu Chai,Ting-Ting Li,Yue Hu,Jinjie Qian,Shaoming Huang
It is of great importance to find non-precious metal based oxygen reduction reaction (ORR) catalysts with high stability, high performance and low cost. In this context, hierarchically porous carbon-based nanomaterials doped with heteroatoms are regarded as one of promising catalysts for ORR. Herein, a bottom-up approach is proposed by using the initial MOF-derived CoO@ZIF-67 core-shell structure as a template to obtain hollow cobalt-anchored N-doped carbon material followed by acid etching ( A-CoNC ). It exhibits a type of hollow porous nitrogen-carbon network anchored by well-dispersed atomic Co-N x sites with high activity and stable catalytic performance. The as-obtained A-CoNC shows high electrocatalytic ORR activity, good reaction selectivity with the low Tafel slope of 55.5 mV dec −1 , large limited current density of 5.37 mA cm −2 and excellent long-term stability (retention = 96.1%, time = 10 h). Furthermore, A-CoNC can also be serving as efficient electrocatalysts for zinc-air battery with a high power density of 144.0 mW cm −2 . Our synthetic strategy from the MOF-derived core-shell structure to ORR electrocatalyst provides new pathway for the design and preparation of highly efficient electro-/photo-catalysts stemmed from MOFs materials.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-13
·
IF 16.6
Luo Huihui,Tian Shuainan,Liang Hongliang,Wang He,Gao Shuang,Dai Wen
The cleavage and functionalization of C–S bonds have become a rapidly growing field for the design or discovery of new transformations. However, it is usually difficult to achieve in a direct and selective fashion due to the intrinsic inertness and catalyst-poisonous character. Herein, for the first time, we report a novel and efficient protocol that enables direct oxidative cleavage and cyanation of organosulfur compounds by heterogeneous nonprecious-metal Co-N-C catalyst comprising graphene encapsulated Co nanoparticles and Co-Nx sites using oxygen as environmentally benign oxidant and ammonia as nitrogen source. A wide variety of thiols, sulfides, sulfoxides, sulfones, sulfonamides, and sulfonyl chlorides are viable in this reaction, enabling access to diverse nitriles under cyanide-free conditions. Moreover, modifying the reaction conditions also allows for the cleavage and amidation of organosulfur compounds to deliver amides. This protocol features excellent functional group tolerance, facile scalability, cost-effective and recyclable catalyst, and broad substrate scope. Characterization and mechanistic studies reveal that the remarkable effectiveness of the synergistic catalysis of Co nanoparticles and Co-Nx sites is crucial for achieving outstanding catalytic performance.
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JOURNAL OF POWER SOURCES
·
2026
·
IF 8.4
Jia Yu,Kaiqiang Xu,Sheng Han
Developing efficient, cost-effective, and durable oxygen reduction reaction (ORR) catalysts to accelerate the sluggish kinetics, is crucial for emerging alkaline fuel cell technologies such as direct ammonia borane fuel cells (DABFCs). Herein, a bimetallic metal–organic framework (MOF)-derived Co-N x /NC catalyst with highly dispersed Co-N x nanoclusters embedded in an N-doped carbon framework is synthesized for enhanced ORR performance. The Co-N x /NC catalyst displays a half-wave potential of 0.86 V vs. RHE in 0.1 M KOH and excellent stability with 99.2% current retention at 0.67 V vs. RHE for 20000 s. When applied in a DABFC single cell, it achieves a peak power density of 33 mW cm −2 at 298 K under low fuel and electrolyte concentrations (1.0 M KOH + 0.1 M AB). Structural characterization and electrochemical analyses suggest that the enhanced ORR activity and stability are associated with highly dispersed Co-N x nanoclusters and pyridinic-N species. This work highlights a bimetallic MOF precursor strategy for developing high-performance ORR catalysts for alkaline fuel cells.
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