CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Shuangxi Lin,Longchen Gong,Ning Zhao,Huibo Zhao,Feigang Zhao,Yang Bai,Zhenhua Li,Wen Liu
Modulating metal-support interactions is critical for improving catalytic activity and product selectivity for CO 2 hydrogenation. Such modulation can be achieved by modifying the metal nanoparticles as well as the supports. Here, we prepared a novel catalyst, in which Ni nanoparticles were dispersed on CeO 2 and hexagonal boron nitride (h-BN) hybrid supports. The introduction of h-BN to Ni/CeO 2 -BN effectively improves the dispersion of Ni nanoparticles. More importantly, the abundant Ni-CeO 2 interfacial sites with enriched oxygen vacancies are formed over h-BN edge sites. The dispersed Ni species are anchored on CeO 2 via a unique interfacial structure, with electron-rich Ni (Ni δ− ) species. At the interfacial sites on Ni/CeO 2 -BN, the synergy between oxygen vacancies and Ni δ− , which enhances CO 2 activation and H 2 dissociation, respectively, renders superior catalytic performance for CO 2 methanation. In situ DRIFTS suggests formate as key rate-limiting intermediates on Ni-CeO 2 sites, while the formation of B-H bonds further promotes hydrogen activation and subsequently the catalytic performance. The modulation of metal-support interactions by spatial confinement effect by BN offers a new paradigm for designing metal/oxide catalysts for chemical transformations that requires bifunctionality as CO 2 hydrogenation.
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Advanced Energy Materials
·
2024
·Vol. 15
·期 3
·2402295
·
IF 24.4
Songshan Zhu,Shimin Ma,Di Song,Sufang He,Yunzhu Wang,Jichang Lu,Tianhao Ai,Yongming Luo
The regulation and stabilization of strong metal-support interactions (SMSI) in high temperature hydrogen-rich reaction condition remains a huge challenge due to its structural sensitivity. Herein, tunable SMSI is constructed and stabilized on TiO 2 supported Ni catalysts by TiO 2 crystal phase engineering strategy, and then a SMSI-degree-depended ethanol stream reforming (ESR) performance is demonstrated. Rutile supported Ni exhibited a weakened SMSI with 48.6% coverage, exposing more metallic Ni and Ni-TiO 2 perimeter interface sites, and displayed exceptional H 2 yield of 4.7 mol H2 /mol ethanol and an ultra-long stability of 420 h without deactivation at 500 °C. The low reaction energy and high resistance to carbon deposition (0.9 mg c /g cat ·h) and Ni 0 sintering on Ni/r-TiO 2 catalyst explained its excellent catalytic performance. Furthermore, the effect of well-defined SMSI structures on the reaction pathway and deactivation mechanism of the ESR is clarified. This work provides a precedent for the tailor and application of SMSI in high temperature hydrogen-rich reaction conditions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
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IF 24.319
Aiqun Kong,Mao Peng,Menghui Liu,Ye Lv,Houjun Zhang,Yusheng Gao,Jing Liu,Yan Fu,Wei Li,Jinli Zhang
Herein, we developed a novel and simple strategy to construct Pt-decorated TiO 2 /β-Ni(OH) 2 nanosheet arrays that steadily deliver large current densities in alkaline electrolyte. It is of great interest to find that the versatile role of few-layered Ti 3 C 2 endows the unique growth mechanism of Pt/TiO 2 /β-Ni(OH) 2 . It is worth noting that the interconnected array electrode exhibits noticeable hydrogen evolution reaction (HER) performance, achieving ultralow overpotentials of 107, 145 and 184 mV at high current densities of 500, 1000 and 1500 mA cm −2 , respectively, which outperforms most reported HER electrocatalysts. It requires only 1.95 V to drive 1000 mA cm −2 towards full water electrolysis along with considerable stability. It is demonstrated for the first time that the synergistic effect of Pt and TiO 2 /Ni(OH) 2 the enhanced HER performance. This work reports a robust nanoarray support for Pt electrocatalyst to break through its intrinsic barrier in alkaline HER and under large current density.
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Nano-Micro Letters
·
2022
·Vol. 14
·期 1
·1-16
·
IF 23.655
Cheng Haoran,Pan Yamin,Wang Xin,Liu Chuntai,Shen Changyu,Schubert Dirk W.,Guo Zhanhu,Liu Xianhu
Ni-MXene/MF foam is synthesized via an electrostatic assembly and dip-coating process.
The “micro-capacitor” structure of Ni/MXene and the 3D porous structure of MF endow the foam excellent impedance matching and wave absorption performance.
The excellent heat insulation, infrared stealth, and flame-retardant performances are achieved.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Xin-jie Zhao,Ying-jie Sun,Wei-hong Chai,Xiao-jing Wang,Jun Zhao,Yu-pei Li,Fa-tang Li
The spatial photoinduced charge separation and atomic H 2 evolution active site is decisive in the operating efficiency of the photocatalytic hydrogen evolution reaction, yet its rational design and synthesis remain a grand challenge. Here, a series of Hofmann-type coordination polymers (HCPs) with planar anionic block [Ni(CN) 4 ] 2- units were found to effectively enhance the photocatalytic H 2 evolution reaction (PHER) activity of transition metal sulfides (TMSs). This proof-of-concept study investigated four HCPs with planar anionic block [Ni(CN) 4 ] 2- units combined with different central transition metal ion (M 2+ : Ni, Co, Fe, and Mn). All four HCP-modified TMSs exhibited remarkable PHER activity of more than 20.0 mmol g −1 ·h −1 and an apparent quantum yield of ∼20 %, surpassing that of optimized Pt/Zn 0.5 Cd 0.5 S by more than 1.5-fold. Through spectroscopic characterization, Kelvin probe force microscopy (KPFM), and density functional theory (DFT) simulations, we confirmed that the [Ni(CN) 4 ] 2- units potentially bridged with the TMSs via an M-S bond forming an electronic transmission channel, thus eliminating the interface energy barrier. Due to the appropriate band structure, the photogenerated electrons converged to the [Ni(CN) 4 ] 2- units, consequently facilitating the conversion of H + to H 2 . This work demonstrates a rational synthetic route for creating PHER photocatalysts that possess mild synthesis conditions, efficient electronic transmission interfaces, and an active center that can be finely manipulated.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Haoran Yin,Ziyan Lin,Lixia Wang,Yong Huang,Tayirjan Taylor Isimjan,Xiulin Yang
Understanding the oxygen evolution reaction (OER) mechanism is critical for the rational design of high-performance OER electrocatalysts. Theoretically, the lattice oxygen oxidation mechanism (LOM) bypassing the inherent limitations of the traditional adsorbate evolution mechanism through direct interactions between lattice oxygen and oxygen intermediates, thereby lowering the energy barrier of alkaline OER. However, effective lattice oxygen activation remains a significant challenge. Herein, a Ni-based metal-organic framework, Ni N x F 10-x , was employed as a model system to precisely regulate the local microenvironment around the Ni active site via the push-pull effect of organic ligand side groups, thus achieving an efficient LOM pathway. Experimental results demonstrated that this electronic push-pull effect induced lattice strain and morphology variations in Ni N x F 10-x , driven to generate more unsaturated metal sites. The optimized Ni N 3 F 7 /CP exhibited excellent OER activity, achieving a low overpotential of 213 mV at 10 mA cm⁻² and long-term stability in 1.0 M KOH. In-situ electrochemical impedance spectroscopy, in-situ Raman, DEMS and density functional theory calculations combined to illustrate that this ligand functionalization significantly benefited the LOM pathway and OER performance by optimizing intermediate adsorption. This work provides a new perspective for developing advanced OER catalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Shihu Cao,Shugang Zheng,Tianci Liu,Jinhao Liu,Yaqi Yin,Dan Feng,Yunqing Liu,Dayi Qian,Jiangwei Shang,Xiuwen Cheng
Herein, we identified interfacial oxygen vacancy-metal (O V -Ni) dual-sites within a NiFe 2 O 4 /Ni@NC composite as the definitive structural origin for dictating the selective evolution of singlet oxygen ( 1 O 2 ) from peroxymonosulfate (PMS) activation. The catalyst was fabricated via in-situ pyrolysis of a Ni-MOF on NiFe 2 O 4 nanoparticles, and its mechanism was elucidated through a combination of in-situ spectroscopy, kinetic analysis, and density functional theory (DFT) calculations. This 1 O 2 -driven catalysis achieved an 11-fold enhancement in the levofloxacin degradation rate, with the interfacial synergy lowering the non-radical pathway’s energy barrier by 0.037 eV. We conclude that these engineered dual-sites deterministically control reaction selectivity, as proven by the first experimental trapping of a surface-bound 1 O 2 precursor. This work establishes a design blueprint for advanced non-radical catalysts by transforming the approach from serendipitous discovery to predictable, interface-driven design.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Weiju Hao,Dongxue Yao,Qiuyu Xu,Ruirui Wang,Chenglong Zhang,Yanhui Guo,Ruimin Sun,Mingxian Huang,Ziliang Chen
The aggregation of transition metal nanoparticles severely degrades their catalytic activity towards water splitting. Although this issue can be alleviated by the popular carbon-hybridization and metal foam-confinement strategies, the complicated fabrication procedure and the support corrosion parasitic in these strategies inevitably result in high usage cost and unsatisfactory cycle durability. Herein, we in-situ space-confined boron-inserted Fe-Ni solid solution nanosheets onto the activated hydrophilic sponge (B-FeNi@HS) via substitution of Fe by Ni and insertion of B within the Fe lattice interstitials in the presence of NH 4 + -modified dimethylamino borane solution. When served as the bifunctional electrocatalysts, B-FeNi@HS only needs overpotentials of 54 and 171 mV to afford 10 mA cm –2 for HER and OER in 1.0 M KOH, respectively. In addition, the alkaline overall-water splitting system constructed by using B-FeNi@HS as two-electrodes only delivers an ultralow cell voltage of 1.456 V to drive 10 mA cm –2 , and shows negligible activity decay even at 500 mA cm –2 for 3 days. Such outstanding performance can be traced to the synergism of corrosion-resistant support, hierarchical morphology with favorable surface area and dual solid-solution crystal structure, ensuring robust mechanical stability, rapid charge/mass transfer kinetics as well as the energetically favorable formation of intermediates during catalysis. The proposed strategy is versatile and can be extended to synthesize other efficient B-inserted Fe-based electrocatalysts.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Steven Hu,Xinghui Liang,Huimin Yuan,Zhenning Xu,Jun Wang,Hai Liu,Kaihua Xu,Xing Ou
The development of Co-free ultrahigh-Ni (Ni > 0.9) layered oxide cathode materials holds immense promise for addressing electric vehicle range limitations and cost efficiency, though substantial obstacles persist in structural durability, thermal stability, and safety. To concurrently enhance the structural integrity and interfacial stability of LiNi 0.95 Mn 0.05 O 2 , a dual-functional co-regulation strategy integrating Zr/Al bulk doping with Li 6 Zr 2 O 7 surface coating is implemented. Controlled Zr 4+ /Al 3+ co-incorporation expands interlayer spacing, strengthens transition metal–oxygen bonding, and stabilizes the oxygen framework, thereby improving Li + diffusion kinetics while suppressing cation disorder. Concurrently, the epitaxially Li 6 Zr 2 O 7 coating effectively passivates the surface by eliminating residual lithium species, inhibiting grain coarsening, and suppressing interfacial side reactions. These coupled bulk-surface modifications synergistically inhibit mechanical stress-induced crack propagation and deleterious phase transformations. Therefore, the optimized cathode achieves 96.9% capacity retention after 100 cycles at 1 C, while maintaining stable operation under extreme electrochemical conditions (4.5 V cutoff voltage) and thermal extremes (−10 °C/60 °C). This work demonstrates a synergistic modification paradigm for designing robust ultrahigh-Ni cathodes, thereby propelling the advancement of next-generation high-energy density lithium-ion batteries.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·Vol. 35
·期 2
·2412895
·
IF 18.5
Dedong He,Yimin Zhang,Tan Li,Dingkai Chen,Hao Wang,Lei Zhang,Jiangping Liu,Xiaohua Cao,Jichang Lu,Yongming Luo
Conversion of CO 2 and CH 4 into syngas offers a promising route to reduce emissions of greenhouse gases, which facilitates large-scale carbon fixation and boosts carbon-neutral goal. The main obstacle for CO 2 /CH 4 reforming is the lack of durable catalysts showing both high metal-exposure and high-temperature structure stability, since the reported Ni-based catalysts have difficulty in avoiding deactivation by sintering metal at high temperature. Herein, ultra-small Ni nanoparticles, which display multiple characteristics of high surface-exposure and stabilized structure, are constructed from the evolution of atomically dispersed low-valent nickel under a dually confined microenvironment. Consequently, the developed strategy can not only break the stable-exposure trade-off in heterogeneous catalysis but also provide new opportunity for the engineering of high-performance and sintering-resistant reforming catalysts as well as other durable heterogeneous catalysts.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Rushuo Li,Tao Ban,Danfeng Zhao,Fajie Hu,Jing Lin,Xiubing Huang,Zhiping Tao,Ge Wang
Defect engineering improves the catalytic performance of metal-organic frameworks (MOFs) loaded metal nanoparticles (MNPs@MOFs), but there is still a challenge in defining the structure-activity relationships. Herein, the content of linker-missing defects in UiO-66(Ce) was systematically regulated via formic acid as the modulators, and defective UiO-66(Ce) loaded Ni nanoparticles (NPs) were constructed for dicyclopentadiene (DCPD) hydrogenation. The fine regulation of defect engineering and reduction conditions affected the structure properties of UiO-66(Ce) and the electronic metal-support interaction between MOFs and Ni NPs, thereby optimizing the microenvironment and electronic state of Ni NPs. The optimized U(Ce)-40eq with suitable defects, small size and structure stability effectively promoted the production of highly dispersed abundant electron-deficient Ni 0 active sites, enhancing the adsorption and activation of H 2 and C=C bonds, especially accelerating the rate-determining step. Therefore, U(Ce)-40eq loaded 5 wt% Ni NPs achieved DCPD saturated hydrogenation to tetrahydrodicyclopentadiene (70 °C, 2 MPa, 90 min), superior to most high-loading Ni-based catalysts. This work reveals the synergistic mechanism of MOFs defect engineering and electronic structure of Ni NPs, providing effective guidance for the precise preparation of highly efficient and stable MNPs@MOFs heterogeneous catalysts.
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高影响因子
ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Jinjing Du,Yu Zhou,Xinhai Liu,Xinxin Cui,Xuan Zhang,Bin Wang,Xiao Feng,Jun Zhu,Heng Zuo,Qian Li,Xihong He,Ping Hu
The development of a hydrogen evolution catalyst with both catalytic activity and stability is critical for hydrogen production from electrolytic water. Herein, a V-based porous alloy was prepared via high-energy ball milling and solid-state sintering. Then, the V-based porous alloy was modified with a Ni-Cu-Mo ternary alloy coating by direct current electrodeposition to obtain a composite hydrogen evolution cathode with high hydrogen evolution activity. The substrate has a certain hydrogen storage capacity combined with a high-activity Ni-Cu-Mo coating. The composite hydrogen evolution cathode exhibited high electrocatalytic activity toward the HER. It can afford a lower overpotential of 93 mV and a smaller Tafel slope of 97.4 mV/dec with a current density of 10 mA/cm 2 in 1.0 M KOH. The composite hydrogen evolution cathode demonstrated outstanding stability after 2000 cycles and good durability after intermittent electrolysis for 20 h. Hydrogen protons can protect the components of the cathode composite from dissolution during discontinuous constant potential electrolysis. The composite hydrogen evolution cathode also exhibited a strong catalytic capacity for hydrogen evolution during intermittent electrolysis under alkaline conditions.
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高影响因子
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