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学者姓名：钟守超
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Abstract ：
Developing novel non-precious metal-based catalysts is crucial to achieving low-cost, stable, and industrial-grade overall water splitting. Although NiSe2 shows significant promise as an electrocatalyst due to its excellent electrical conductivity and stability in acidic and alkaline environments, its performance is limited by inherently poor activity. In this study, a nanorod-shaped CoxNi1-xSe2@Co(OH)2/nickel foam (CNSC/NF) alkaline water-splitting catalyst was constructed in situ through a hydrothermal-gamma radiation method. The gamma radiation imparted NiSe2 with an "island-like" amorphous/crystalline heterostructure and a high density of atomic-level Ni-Se-Co electron bridge structures. The dense "ball-stick" configuration and heterointerfaces in CNSC/NF jointly enhanced structural stability for ampere-level water splitting. CNSC/NF achieved a current density of 1 A cm-2 at a cell voltage of only 2.15 V for over 1000 h under rigorous working conditions. Experimental and theoretical analyses revealed that the amorphous Ni-Se-Co electron bridges triggered asymmetric d-p-d orbital hybridization via electron-directed transfer, effectively facilitating H2O dissociation and adsorption for *H/*OOH intermediates. The rapid oxidative reconstruction of active Ni-Se-Co sites further improved the intrinsic activity. This work proposes a convenient strategy to fabricate an efficient, durable NiSe2-based catalyst and provides insights into the effects and evolution of amorphous atomic doping during water-splitting process.
Keyword ：
Alkaline water splitting Alkaline water splitting Amorphous heterostructure Amorphous heterostructure Anion exchange membrane electrolyzer Anion exchange membrane electrolyzer Atomic doping Atomic doping Nickel selenide Nickel selenide
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| GB/T 7714 | Jiang, Fan , Wang, Yicheng , Peng, Haoyu et al. Triggering asymmetric hybridization via Ni-Se-Co electron bridges on rich amorphous heterostructured nickel selenide for durable alkaline water splitting [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2025 , 372 . |
| MLA | Jiang, Fan et al. "Triggering asymmetric hybridization via Ni-Se-Co electron bridges on rich amorphous heterostructured nickel selenide for durable alkaline water splitting" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 372 (2025) . |
| APA | Jiang, Fan , Wang, Yicheng , Peng, Haoyu , Wu, Yiqian , Zhang, Zeyu , Li, Yichen et al. Triggering asymmetric hybridization via Ni-Se-Co electron bridges on rich amorphous heterostructured nickel selenide for durable alkaline water splitting . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2025 , 372 . |
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Capture of acid gases holds crucial importance for addressing air pollution and climate change, where achieving a molar ratio for adsorption and separation of acid gases on an active site higher than 1.0 remains challenging. Herein, we demonstrate that three nitrogen-bonded one Zn sites within a single-crystalline-like porous carbon (Zn-N3@SC-PC) derived from controlled carbonization of ZIF-8-C equivalent to N with KCl, exhibit supra-multi-molar adsorption for CO2, COS, and H2S, even to 1:6 ratio for SO2 on the Zn-N3. This exceptional performance is attributed to the protruded structure in the Zn-N3@SC-PC for more coordination between Zn vacant orbital and acid gases evidenced by DFT calculation and in situ EXAFS. The high capacity for capturing acid gases on this adsorbent is crucial for future in carbon neutrality and environment protection.
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| GB/T 7714 | Zhang, Guanqing , Liu, Fengqing , Zhong, Shouchao et al. Surpassing stoichiometric limitation for supra-multi-molar adsorption and separation of acid gases [J]. | NATURE COMMUNICATIONS , 2025 , 16 (1) . |
| MLA | Zhang, Guanqing et al. "Surpassing stoichiometric limitation for supra-multi-molar adsorption and separation of acid gases" . | NATURE COMMUNICATIONS 16 . 1 (2025) . |
| APA | Zhang, Guanqing , Liu, Fengqing , Zhong, Shouchao , Liu, Fujian , Zhu, Qiliang , Tang, Yu et al. Surpassing stoichiometric limitation for supra-multi-molar adsorption and separation of acid gases . | NATURE COMMUNICATIONS , 2025 , 16 (1) . |
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Trace ammonia reversible adsorption and sieving using solid adsorbents present a critical challenge in the practical deployment of ammonia-hydrogen fuel cells. Herein, we design porous polydivinylbenzene (P-PDVB) through one-pot solvothermal polymerization without additional templates. Subsequently, solvent-induced network swelling was performed to achieve deep sulfonation of the P-PDVB using chlorosulfonic acid, resulting in P-PDVB-SO3H-x, which possess large specific surface areas, abundant micro-mesoporosity, and high acid site densities. Notably, P-PDVB-SO3H-x demonstrate superior performance for the selective capture and sieving of NH3 from an N2/H2/NH3 mixture, outperforming most previously reported NH3 adsorbents. Thus, P-PDVB-SO3H-x can serve as an efficient adsorbent for the selective removal of trace ammonia from ammonia-hydrogen fuel cell systems, significantly improving both the efficiency and longevity of the fuel cells. This work highlights the potential of P-PDVB-SO3H-x as a promising candidate for enhancing ammonia-hydrogen fuel cell performance, paving the way for further exploration of advanced adsorbent materials in energy applications.
Keyword ：
ammonia-hydrogen fuel cell ammonia-hydrogen fuel cell ammonia separation ammonia separation deep sulfonation deep sulfonation porous organic polymers porous organic polymers selective adsorption selective adsorption solvothermal synthesis solvothermal synthesis
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| GB/T 7714 | Qu, Yongfang , Zhang, Wentao , Zhong, Shouchao et al. Reversible adsorption and sieving of trace NH3 from NH3-H2 fuel cells systems using sulfonated porous polydivinylbenzene [J]. | AICHE JOURNAL , 2025 , 71 (5) . |
| MLA | Qu, Yongfang et al. "Reversible adsorption and sieving of trace NH3 from NH3-H2 fuel cells systems using sulfonated porous polydivinylbenzene" . | AICHE JOURNAL 71 . 5 (2025) . |
| APA | Qu, Yongfang , Zhang, Wentao , Zhong, Shouchao , Zhuo, Linyu , Wang, Xi , Fang, Huihuang et al. Reversible adsorption and sieving of trace NH3 from NH3-H2 fuel cells systems using sulfonated porous polydivinylbenzene . | AICHE JOURNAL , 2025 , 71 (5) . |
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Herein, a variety of 2,6-diaminopyridine (DAP) derived nitrogen-doped hierarchically porous carbon (DAP-NHPC-T) prepared from carbonization-induced structure transformation of DAP-Zn-SiO2-P123 nanocomposites are reported, which are facilely prepared from solvent-free co-assembly of block copolymer templates P123 with pyridine-rich monomer of DAP, Zn(NO3)2 and tetramethoxysilane. In the pyrolysis process, P123 and SiO2 templates promote the formation of mesoporous and supermicroporous structures in the DAP-NHPC-T, while high-temperature volatilization of Zn contributed to generation of micropores. The DAP-NHPC-T possess large BET surface areas (≈956–1126 m2 g−1), hierarchical porosity with micro-supermicro-mesoporous feature and high nitrogen contents (≈10.44–5.99 at%) with tunable density of pyridine-based nitrogen sites (≈5.99–3.32 at%), exhibiting good accessibility and reinforced interaction with SO2. Consequently, the DAP-NHPC-T show high SO2 capacity (14.7 mmol g−1, 25 °C and 1.0 bar) and SO2/CO2/N2 IAST selectivities, extraordinary dynamic breakthrough separation efficiency and cycling stability, far beyond any other reported nitrogen-doped metal-free carbon. As verified by in situ spectroscopy and theoretical calculations, the pyridine-based nitrogen sites of the DAP-NHPC-T boost SO2 adsorption via the unique charge transfer, the adsorption mechanism and reaction model have been finally clarified. © 2024 Wiley-VCH GmbH.
Keyword ：
charge transfer charge transfer hierarchical porosity hierarchical porosity pyridine-based nitrogen sites pyridine-based nitrogen sites SO2 capture SO2 capture triple template directed synthesis triple template directed synthesis
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| GB/T 7714 | Zhang, G. , Liu, F. , Zhu, Q. et al. Triple Templates Directed Synthesis of Nitrogen-Doped Hierarchically Porous Carbons from Pyridine Rich Monomer as Efficient and Reversible SO2 Adsorbents [J]. | Small , 2024 , 20 (46) . |
| MLA | Zhang, G. et al. "Triple Templates Directed Synthesis of Nitrogen-Doped Hierarchically Porous Carbons from Pyridine Rich Monomer as Efficient and Reversible SO2 Adsorbents" . | Small 20 . 46 (2024) . |
| APA | Zhang, G. , Liu, F. , Zhu, Q. , Qian, H. , Zhong, S. , Tan, J. et al. Triple Templates Directed Synthesis of Nitrogen-Doped Hierarchically Porous Carbons from Pyridine Rich Monomer as Efficient and Reversible SO2 Adsorbents . | Small , 2024 , 20 (46) . |
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Ordered mesoporous carbon@silica hybrid frameworks with high nitrogen content and good stabilities show great significance to improve their functionalities. Herein, we report novel nitrogen-doped (3.51 - 4.62 wt%) and ordered mesoporous carbon@silica frameworks (N-OMC@SiO2) with reinforced nitrogen stability. The NOMC@SiO2 were designed from tricomponent direct co-assembly between block copolymer template and mixed precursors containing urea and tetramethoxysilane without using additional solvent. The N-OMC@SiO2 have large BET surface areas (444.3 - 674.9 m2/g), uniform mesoporous channels (5.8 - 10.9 nm) with well-defined hexagonal symmetry, and stable carbon@silica "reinforced concrete" framework that can be transformed into carbon@silicon by controllable reduction. The nitrogen sites were firmly embedded into their frameworks via the formation of Si-N bonding. Thus, the resulted N-OMC@SiO2 exhibit multi-functionalities and enhanced recyclability in acid waste gas capture and gaseous sulfides catalytic utilization, better than many reported porous adsorbents and catalysts. This study may help develop stable and efficient N-OMCs nanocomposites for acidic gas selective removal.
Keyword ：
Acid gas selective capture Acid gas selective capture Carbon@silica composites Carbon@silica composites Gaseous sulfides elimination Gaseous sulfides elimination Nitrogen -doping Nitrogen -doping Ordered mesoporosity Ordered mesoporosity Solvent -free synthesis Solvent -free synthesis
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| GB/T 7714 | Kan, Xun , Liu, Zihao , Sun, Yafei et al. Tricomponent direct co-assembly to nitrogen-doped, ordered mesoporous carbon@silica frameworks with enhanced nitrogen stability and multi-functionalities [J]. | CHEMICAL ENGINEERING SCIENCE , 2024 , 292 . |
| MLA | Kan, Xun et al. "Tricomponent direct co-assembly to nitrogen-doped, ordered mesoporous carbon@silica frameworks with enhanced nitrogen stability and multi-functionalities" . | CHEMICAL ENGINEERING SCIENCE 292 (2024) . |
| APA | Kan, Xun , Liu, Zihao , Sun, Yafei , Zhong, Shouchao , Zheng, Yong , Liang, Shijing et al. Tricomponent direct co-assembly to nitrogen-doped, ordered mesoporous carbon@silica frameworks with enhanced nitrogen stability and multi-functionalities . | CHEMICAL ENGINEERING SCIENCE , 2024 , 292 . |
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Abstract ：
Herein, a variety of 2,6-diaminopyridine (DAP) derived nitrogen-doped hierarchically porous carbon (DAP-NHPC-T) prepared from carbonization-induced structure transformation of DAP-Zn-SiO2-P123 nanocomposites are reported, which are facilely prepared from solvent-free co-assembly of block copolymer templates P123 with pyridine-rich monomer of DAP, Zn(NO3)(2) and tetramethoxysilane. In the pyrolysis process, P123 and SiO2 templates promote the formation of mesoporous and supermicroporous structures in the DAP-NHPC-T, while high-temperature volatilization of Zn contributed to generation of micropores. The DAP-NHPC-T possess large BET surface areas (approximate to 956-1126 m(2) g(-1)), hierarchical porosity with micro-supermicro-mesoporous feature and high nitrogen contents (approximate to 10.44-5.99 at%) with tunable density of pyridine-based nitrogen sites (approximate to 5.99-3.32 at%), exhibiting good accessibility and reinforced interaction with SO2. Consequently, the DAP-NHPC-T show high SO2 capacity (14.7 mmol g(-1), 25 degrees C and 1.0 bar) and SO2/CO2/N-2 IAST selectivities, extraordinary dynamic breakthrough separation efficiency and cycling stability, far beyond any other reported nitrogen-doped metal-free carbon. As verified by in situ spectroscopy and theoretical calculations, the pyridine-based nitrogen sites of the DAP-NHPC-T boost SO2 adsorption via the unique charge transfer, the adsorption mechanism and reaction model have been finally clarified.
Keyword ：
charge transfer charge transfer hierarchical porosity hierarchical porosity pyridine-based nitrogen sites pyridine-based nitrogen sites SO2 capture SO2 capture triple template directed synthesis triple template directed synthesis
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| GB/T 7714 | Zhang, Guanqing , Liu, Fengqing , Zhu, Qiliang et al. Triple Templates Directed Synthesis of Nitrogen-Doped Hierarchically Porous Carbons from Pyridine Rich Monomer as Efficient and Reversible SO2 Adsorbents [J]. | SMALL , 2024 , 20 (46) . |
| MLA | Zhang, Guanqing et al. "Triple Templates Directed Synthesis of Nitrogen-Doped Hierarchically Porous Carbons from Pyridine Rich Monomer as Efficient and Reversible SO2 Adsorbents" . | SMALL 20 . 46 (2024) . |
| APA | Zhang, Guanqing , Liu, Fengqing , Zhu, Qiliang , Qian, Hao , Zhong, Shouchao , Tan, Jingze et al. Triple Templates Directed Synthesis of Nitrogen-Doped Hierarchically Porous Carbons from Pyridine Rich Monomer as Efficient and Reversible SO2 Adsorbents . | SMALL , 2024 , 20 (46) . |
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A solid ionic liquid adsorbent, obtained by grafting [C3N][SO4H] onto porous carbon was reported. Characterizations including IR, XPS and TEM provided the structural information of the sulfonic acid groups on the porous carbon matrix, affirming the feasibility of this synthesis method. The results elucidated the synergy between the sulfonic acid groups and the pore structure of porous carbon, resulting in substantial enhancements in both ammonia adsorption capacity and adsorption selectivity. Moreover, this absorbent exhibited the ability to capture minute concentrations of ammonia below 0.1 ppm with great efficacy and excellent regeneration property within 8 cycles. This simple grafting and acid activation technique proffers a valuable tool for designing adsorbent of trace ammonia within ammonia-hydrogen fuel cells.
Keyword ：
Ammonia fuel cells Ammonia fuel cells Porous carbon Porous carbon Solid ionic liquids Solid ionic liquids Trace ammonia capture Trace ammonia capture
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| GB/T 7714 | Zhu, Qiliang , Zhang, Wentao , Zhong, Shouchao et al. Precisely capture trace ammonia from fuel cell system over ionic liquid grafted hierarchically porous carbons [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 483 . |
| MLA | Zhu, Qiliang et al. "Precisely capture trace ammonia from fuel cell system over ionic liquid grafted hierarchically porous carbons" . | CHEMICAL ENGINEERING JOURNAL 483 (2024) . |
| APA | Zhu, Qiliang , Zhang, Wentao , Zhong, Shouchao , Xiao, Yao , Qian, Hao , Zheng, Anmin et al. Precisely capture trace ammonia from fuel cell system over ionic liquid grafted hierarchically porous carbons . | CHEMICAL ENGINEERING JOURNAL , 2024 , 483 . |
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