CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Jianlong Wang,Honglin Yan,Cheng Wei,Yuan Ha,Weidong Zhu,Lu Li,Chaoyi Zhou,Qianxin Xiang,Zhimin Li,Yue Hao
Ultra-high Ni layered cathodes LiNi x Mn 1- x O 2 ( x > 0.9) with high energy density for lithium-ion batteries suffer from severe fatigue failure upon cycling because of the unstable crystal structures at highly delithiated states. Despite efforts to address this issue, enhancing the structural stability by electrostatic interaction between oxygen layers has been overlooked. Herein, we propose an electrostatic interaction strategy via Mn-Mg-Al-Ti medium-entropy doping to improve the fatigue resistance of the crystal structure. As expected, these chosen dopants efficiently impede the distortion, interlacement, and fracture of transition metal slabs in crystal structures by enhancing the electrostatic interaction. Accordingly, the cathode LiNi 0.93 Mn 0.04 Mg 0.01 Al 0.01 Ti 0.01 O 2 delivers superior cycling performance with a capacity retention of 96.1 % at 0.5C after 100 cycles. This work demonstrates the effectiveness of improving the electrochemical performance of ultra-high Ni cathodes by the electrostatic interaction strategy, which is of great significance for their commercial application.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Zhao Xin,Li Changzhi,Wen Jie,Qiang Qian,Shen Zirong,Yu Haipeng,Zhou Xin,Yue Fengxia,Fang Ruiqi,Li Yingwei,Zhang Tao
Lignin refining still suffers from great challenges of selective depolymerization and cleavage of stubborn C‒C linkages. Here, a robust atomically dispersed Cu/Ni-SA@HNC catalyst is fabricated for super-selective hydrogenolysis of lignin and model compounds via an unusual “preferential C α –C β bond cleavage in β-O-4 linkages” pathway, affording toluene in yield up to 75.7% from β-O-4 model compounds, and up to 33.7 ± 1.6 wt% (nine parallel experiments) from poplar lignin. The catalyst exhibits high stability, and the scale-up potential is demonstrated by the high space-time yield of toluene (33.7 g·g cat −1 ·h −1 ) in continuous flow reaction of β-O-4 model compound. The origin of the extraordinary selectivity towards C α –C β bond cleavage rather than C‒O bond cleavage in β-O-4 model compounds is uncovered. This work conquers the major challenges in lignin valorization by using non-noble dual-metal single-atom catalyst, not only showcasing the application perspective of atomically dispersed catalysts in biopolymer refinery, but also providing a cost-efficient, petroleum independent solution to valuable commodity chemicals.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Yi-Ran Du,Rui Wang,Qing-Shan Niu,Yi-Yu Tao,Bao-Hua Xu
In this study, the bimetallic RuM-CeO 2 (M = Ni, Fe, Cu, K and Cs) catalysts were facilely fabricated by taking the commercially available CeO 2 (99.95 % metals basis, Aladdin, < 50 nm of diameter) as the support. They displayed distinct catalytic performance, especially the chemo-selectivity, on the methoxycarbonylation of styrene with CO and CH 3 OH. Impressively, Ru 2 Ni 0.6 -CeO 2 provided an up to 90.1 % yield of methyl phenylpropionate with satisfied linear selectivity (L/B = 91/9). The characterization and mechanistic results demonstrated that the doping of proper amount of Ni species enriches the local oxygen vacancy (Vö) at the surface but slightly reduces the charge at Ru sites, thereby modulating the interfacial Lewis acid − base pair (Ru-O-Ce-Vö) for catalysis. It thus enhances the CH 3 OH dissociation, leading to high coverage of OCH 3 species with low adsorption energy and relatively weak acidity. Further, the insertion of CO becomes readily due to the weak Ru-CO affinity at electron-deficient Ru center therein. As such, the apparent activation energies ( E a ) of styrene methoxycarbonylation over Ru 2 -CeO 2 (71.2 kJ mol −1 ) is nearly half-reduced by doping Ni element (Ru 2 Ni 0.6 -CeO 2 : 37.5 kJ mol −1 ). Meanwhile, the competitive side reactions at the surface of Ru 2 Ni 0.6 -CeO 2 is inhibited without sufficient acid strength and acid sites. Both aromatic olefins and cyclic olefins were well tolerated under such a system.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Pei Liu,Haoran Wei,Tao Huang,Zhencheng Huang,Lingli Chen,Xuanlong He,Yuying Liu,Hongkai Yang,Mijie Liu,Shenghua Ye,Xuming Yang,Zhanhua Wu,Yaming Liu,Qingqing Jia,XiaoBai Ma,Jing Chen,Xiangzhong Ren,Xiaoping Ouyang,Jianhong Liu,Qianling Zhang,Jiangtao Hu
Ni-rich single-crystalline layered cathodes have garnered significant attention due to their high energy density and thermal stability. However, they experience severe capacity degradation caused by lattice strain and interfacial side reactions during practical applications. In this study, an effective yttrium modification method is employed to stabilize the structure of Ni-rich single-crystalline LiNi0.83Mn0.05Co0.12O2 (SC-NMC83) to solve these issues. This innovative approach successfully immobilizes oxygen within the material, preventing crack formation while simultaneously broadening the diffusion path of Li+. The yttrium-modified sample (SC-NMC83-Y) exhibits a superior capacity retention compared to the SC-NMC83 sample, with values of 90% and 76.1% after 100 cycles, respectively. This work demonstrates the promising potential of a doping strategy for Ni-rich single-crystalline cathodes and paves a pathway for its practical implementation, such as all-solid-state batteries.
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JOURNAL OF MOLECULAR STRUCTURE
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2024
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IF 4
Hongyan Zhang,Xuehan Yang,Hua Wang,Yikai Wang,Ranran Li,Heye Fu,Hao Zhou,Dan Wu,Pan Yuang,Maoshuai He,Wenxian Wei,Tao Yang
Hydrogen has long been widely recognized as a promising carbon-free fuel with potential to tackle energy and environmental challenges owing to its high energy density and cleanliness. Water electrolysis offers an environmentally friendly method for hydrogen production from water and largely depends on the efficiency of electrocatalysts. Molybdenum diselenide (MoSe 2 ) has been regarded as one of the most promising earth-abundant and cost-effective catalysts for hydrogen evolution reaction (HER). Nevertheless, its catalytic activity has thus far remained below expectations. In this research, we introduce a vanadium-modulated Ni-MoSe 2 catalyst (NiV-MoSe 2 ), demonstrating outstanding catalytic performance towards HER with an overpotential of 74.5 mV at 10 mA cm −2 and a Tafel slope of 56.2 mV dec −1 . The enhancement of catalytic performance is highly likely attributed to the dual doping of vanadium and nickel. As a result, the intrinsic activity, electrochemical active surface area, and conductivity are significantly improved. These findings enable the NiV-MoSe 2 catalyst to be an exceptionally competitive alternative to noble metal-based catalysts, and may stimulate further studies in designing efficient HER catalysts through multi-heteroatom substitution.
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Catalysts
·
2024
·Vol. 14
·期 11
·756
·
IF 3.8
Xuekai Shan,Guolin Zhang,Ying Zhang,Shuobo Zhang,Fang Guo,Qi Xu
Selective CO2hydrogenation faces significant technical challenges, although many efforts have been made in this regard. Herein, a Ni-doped In2O3catalyst supported by g-C3N4was prepared using the co-precipitation method, and its composition, morphology, specific surface area, and band gap were characterized using TEM, XPS, BET, XRD, CO2-TPD, H2-TPR, UV-Vis, etc. The catalytic hydrogenation reduction of CO2to produce methanol was tested. Under low-photothermal conditions (1.0 MPa), the hydrogenation of carbon dioxide to methanol is stable, effective, and highly selective, with a spatiotemporal yield of 86.0 gMeOHh−1kgcat−1, which is 30.9% higher than that of Ni-In2O3without g-C3N4loading under the same conditions.
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Catalysts
·
2025
·Vol. 15
·期 9
·886
·
IF 4
Qianran Feng,Xiaoting Yu,Jinlian Peng,Siying Du,Liuyun Chen,Xinyuan Xu,Tongming Su
Sustainable production of hydrogen is currently a global research hotspot. In this study, a Ni(OH)2cocatalyst was loaded on Zn0.8Cd0.2S to form Ni(OH)2/ZCS composites and achieve highly efficient photocatalytic hydrogen production. After Ni(OH)2loading, a close contact interface was established between Ni(OH)2and Zn0.8Cd0.2S, which increased the separation efficiency of the photogenerated electrons and holes. Moreover, the addition of Ni(OH)2increases the specific surface area and light absorption of Ni(OH)2/Zn0.8Cd0.2S, and the Ni(OH)2can act as active sites for photocatalytic hydrogen production. The photocatalytic H2production rate of Ni(OH)2/ZCS composites increases with the increase in the Ni amount. 9Ni(OH)2/ZCS exhibited the optimum H2production rate of 12.88 mmol h−1g−1, which was 9.9 times higher than that of Zn0.8Cd0.2S. When the amount of Ni(OH)2is further increased, the excess Ni(OH)2covers the active site of Zn0.8Cd0.2S and reduced the light absorption of Zn0.8Cd0.2S, resulting in a decrease in the H2production rate. Furthermore, the H2production rate of 9Ni(OH)2/ZCS decreased from 12.88 to 5.15 mmol g−1h−1after 3 cycles. The main reason for the decline in the photocatalytic performance of Ni(OH)2/ZCS is the photocorrosion of Zn0.8Cd0.2S. This study provides an innovative design for loading Ni(OH)2cocatalysts on Zn0.8Cd0.2S to improve the performance of photocatalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Zhihe Zhang,Zihang Yu,Kai Feng,Binhang Yan
CO 2 methanation is gaining renewed attention due to the emerging application needs such as the power-to-gas concept and long-term space exploration missions. Maximizing the amounts of interfacial sites generally regarded as the efficient active sites is considered to be one of the most direct means to enhance catalytic activity but few breakthroughs have been made. Here, Eu 3+ is introduced to Ni/CeO 2 to promote the Ni-CeO 2 interaction, resulting in a remarkable low-temperature CO 2 methanation activity. Structural characterization indicates that the Ni/CeEu(9:1) catalyst achieves higher Ni dispersion compared to Ni/CeO 2 , which consequently generates more interfacial sites. More interfacial sites enhance the proportions of bidentate carbonates closer to interfacial sites as a faster hydrogenated species during the catalytic process, leading to enhanced low-temperature CO 2 methanation activity over the Ni/CeEu(9:1) catalyst. This work provides a chemical strategy to enhance the amounts of active sites and bring insights into the origin of enhanced catalytic performance.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
·
IF 6.3
Ruifeng Xu,Ke Wang,Jiaxin Liu,Zhongkang Cao,Wenbo Wang,Xu Zhang,Bingjun Yang,Juan Yang,Xianfeng Fan,Tongtong Yu,Pengjun Ma
The replacement of the oxygen evolution reaction (OER) with the urea oxidation reaction (UOR) coupled with the hydrogen evolution reaction (HER) in water electrolysis systems is regarded as a highly promising strategy for reducing hydrogen production energy consumption, enhancing hydrogen efficiency, and even effectively treating urea wastewater. However, the design and fabrication of UOR catalysts in the UOR coupled HER catalytic water electrolysis system remains one of the significant challenges. Herein, we employed a facile, operable, and practical solid-state reaction method to synthesize two representative types of transition metal phosphosulfide (MPS 3 ) catalysts, and the intrinsic and structural characteristics of these catalysts were systematically characterized. Subsequently, the MPS 3 catalyst was deposited onto a nickel foam substrate (NF) to obtain the MPS/NF catalytic electrode. The UOR and OER performance of the MPS 3 /NF catalytic electrode was evaluated to elucidate the competitive mechanisms of UOR and OER within the MPS 3 catalyst. Results indicated that the UOR driving potentials required for NiPS 3 /NF and FePS 3 /NF electrodes were individually reduced by 101 mV and 33 mV compared to the corresponding OER driving potentials under the condition of 100 mA/cm 2 , and NiPS 3 /NF and FePS 3 /NF electrodes could even achieve large UOR current density of 300 mA/cm 2 at potentials as low as 1.630 V (vs. RHE) and 1.647 V (vs. RHE), respectively. In-situ Raman spectroscopy combined with XPS analysis revealed distinct catalytic pathways for NiPS 3 and FePS 3 . During catalysis, NiPS 3 undergoes surface reconstruction to form γ-NiOOH, which exhibited superior selectivity toward urea oxidation, whereas FePS 3 predominantly generated β-FeOOH, whose activity was compromised by competing oxygen evolution, thereby conferring weaker UOR selectivity compared with NiPS 3 . For the UOR-coupled HER whole-cell urea electrolysis assessment, the NiPS 3 /NF and FePS 3 /NF whole-cell attained urea degradation efficiencies of 89.04 % and 69.61 %, respectively. This work provided a novel strategy and practical approach for the development of novel, efficient, and cost-effective MPS 3 catalysts for UOR coupled with HER in the treatment of urea wastewater for synergistic hydrogen production.
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CRYSTENGCOMM
·
2025
·
IF 2.6
Wei Jia,Qi He,Zhiqiang Guo,Xiang Wu
It is very important to rationally design electrode materials with remarkable electrical conductivity and high specific surface area for supercapacitors. However, it is limited by insufficient energy density, so the development of high-performance electrodes has become research focuses. Herein, we report the synthesis of CoMoO4@Ni(OH)2 composite structures by hydrothermal growth of Ni(OH)2 nanosheets on CoMoO4 materials. The synthesized product achieves 93% of capacitance retention after 10,000 times cycling and possesses a specific capacitance of 2640 F g-1 at 1 A g-1. Furthermore, the assembled device delivers an energy density of 74.25 Wh kg-1 when the power density is 2700 W kg-1. Besides, the materials still present outstanding flexibility and mechanical stability after bending at different angles and times.
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Rongwei Xu,Guangxu Yao,Shicheng Xu,Danhong Li,Huijuan Zhang,Yu Wang
The rational design of single-atom catalysts (SACs) with tailored coordination environments is essential for improving their electrocatalytic efficacy. This study employs a coordination engineering approach to immobilize atomically dispersed nickel atoms on nitrogen-doped carbon nanofibers (NCNFs), forming a novel Ni–N2O2/NCNFs catalyst. Unlike the traditional Ni–N4 coordination configuration, each nickel atom in this Ni–N2O2 framework is stabilized within a rare and well-defined N2O2 coordination environment. This distinctive local structure is conclusively characterized using single-crystal X-ray diffraction and X-ray absorption spectroscopy. Consequently, the Ni–N2O2/NCNFs catalyst exhibits remarkable hydrogen evolution reaction activity in a 1.0 M KOH solution, necessitating an overpotential of merely 37 mV to attain a current density of 10 mA cm–2. These results confirm the broad-scale applicability of the strategy for modulating the local coordination chemistry of SACs and provide novel insights that will facilitate the design of highly efficient and stable catalysts for alkaline water splitting.
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AICHE JOURNAL
·
2025
·
IF 4
Hong-Da Zhang,Wei-Yao Yang,Miao Pang,Ya-Qiao Tian,Shi-Chao Su,Zhi-Ping Zhao,Le Sang
Non-modified Pd/PDA/Ni foam, hydrophobic modified F 9 -Pd/PDA/Ni foam, and F 17 -Pd/PDA/Ni foam catalysts are successfully prepared and used for NB hydrogenation in micropacked bed reactors (μPBRs). The catalytic performance increases with the addition of water in the water–methanol mixed solvent. In the mixed solvent with 50 v/v% water, F 17 -Pd/PDA/Ni foam can almost completely convert nitrobenzene (NB) with a yield of 95.9% at a mild 45°C. As the solvent contact angle of catalysts increases (87.5–141.5°), the enhancement ratios of NB conversion and AN yield are 28.9%–92.4% and 31.4%–106.5%, respectively. The space–time yield of AN in μPBRs reaches 1.873 kg·L −1 ·h −1 ·g −1 , which is 1–2 orders of magnitude higher than that of conventional reactors. The kinetic model of NB hydrogenation is established at the water–methanol system in μPBRs. The hydrophobicity of catalysts significantly improves the reaction rate of NB hydrogenation, and the reaction rate constant is increased by 69.9%.
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