APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Qiang Fang,Lu Hao,Tao Zhao,Jiahui Li,Genyan Hao,Guang Liu,Dazhong Zhong,Jinping Li,Qiang Zhao
The electrocatalytic production of 2,5-furandicarboxylic acid (FDCA) via the 5-hydroxymethylfurfural oxidation reaction (HMFOR) is an effective and more suitable alternative to the oxygen evolution reaction (OER) in electrocatalytic water splitting. High-valence Ni(III) is critical for the HMFOR, but the formation is greatly limited by the difficult in situ self-oxidation. In this study, the pre-oxidization-derived amorphous NiO x H y nanosheet presents more accessible Ni(III) for efficient HMFOR. In addition, NiO x H y /NF exhibits a low onset potential of 1.35 V, a high FDCA yield of 98.5 %, and a high Faradaic efficiency of 98.3 % for the HMFOR in 0.1 M KOH with 10 mM HMF. In situ Raman spectroscopy results indicate that Ni(III)OOH is an active intermediate in the electrochemical HMFOR. This work provides a strategy for promoting the formation of high-valence Ni(III) and boosting biomass oxidation.
研究领域:
材料科学
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电化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yang Zong,Wenjie Ji,Yu Xie,Deli Wu
The mineralization of organic pollutant by O 3 is prone to be restricted by the accumulative production of oxalate (OA) that is recalcitrant to the attack of hydroxyl radical ( OH). Herein, it was interestingly found that the presence of 0.5 mM Ni(II) enhanced the mineralization efficiency of EDTA by O 3 under alkaline conditions by 22.8%, with the promoting effect of Ni(II) augmented as the increasing loading of Ni(II). Based on the results from scavenging experiment, chemical probe detection and XPS characterization, it was verified that except for the commonly recognized reactive oxidants (i.e., OH and O 3 ) in EDTA mineralization, the overlooked Ni(III) species (i.e., NiOOH) also played an indispensable role in enhancing the mineralization of EDTA. The Ni(III) species was formed via the oxidation of decomplexed Ni(II) by OH and in turn collaborated with OH to decompose EDTA. More importantly, the generated Ni(III) species exerted higher affinity towards OH and O 3 -resistent oxalate, hence elevating EDTA mineralization. This study elucidated the significant role of Ni(III) species in promoting the mineralization efficiency of EDTA, and also proposed a new insight into elevating the treatment performance of ozonation via the collaborative oxidation mechanism-co-mediated by OH and Ni(III) species.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Xin Huang,Xujie Zhou,Shaohong Han,Jizhi Zhou,Guangren Qian,Naiyun Gao
Peroxydisulfate (PDS) activation has attracted much attention for the treatment of drinking water systems. In this work, Ni-doped MgAl layered double hydroxides (Ni-LDHs, Ni:Mg = 1:100 to 1:1, molar ratio) were prepared for the activation of PDS via intercalation. Compared with the case without Ni, doping with Ni resulted in much higher phenol degradation at the same PDS dosage. This was attributed to the activation of PDS, as the PDS consumption increased with increasing Ni doping amount. Moreover, radicals corresponding to organic decomposition were detected in the presence of Ni. Physical characterization results reveal that Ni(II) was converted to Ni(III) with PDS and then reduced back to Ni(II) during organic decomposition. To our best knowledge, this is the first study to report a cycle of Ni(II)-Ni(III)-Ni(II) in LDHs for the efficient activation of PDS. This effect was also observed in cases of odorous substances such as 4-bromophenol, 2-methylisoborneol, and geosmin. Our work provides a promising approach for the activation of PDS by Ni-LDHs.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
POLYMER DEGRADATION AND STABILITY
·
2025
·
IF 7.4
Xiaoyuan Liu,Jia Liu,Xinyi Bao,Wenqing Ge,Zhihui Lv,Li Dang
To overcome the critical challenges of high smoke toxicity and flammability in flexible polyvinyl chloride (fPVC), this study developed a core-shell flame retardant (MOSw@PDA@NiOOH) via polydopamine (PDA) interfacial engineering and in-situ NiOOH deposition on magnesium oxysulfate whiskers (MOSw). SEM, TEM, and EDS confirm the hierarchical interface structure with Ni(III)-based NiOOH nanoparticles uniformly anchored on MOSw surfaces. Cone calorimetry tests show a 35.38% reduction in peak smoke production rate and a 75.88% decrease in total smoke production, respectively, for fPVC/MOSw@PDA@NiOOH compared to fPVC/MOSw composite, along with a UL-94 V-0 rating and 28.8% limiting oxygen index. Raman, TGA, and XPS analyses reveal that: i) the strong Lewis acidity of Ni(III) facilitates chloride elimination from PVC, leading to the formation of conjugated polyene structures; ii) the powerful oxidizing capability of Ni(III) directly oxidizes unsaturated carbons such as C=C, generating carbocations that subsequently promote aromatization and cross-linking reactions; iii) Ni(III) induces complete decomposition of MOSw into MgO, ultimately forming a dense carbonaceous residue layer composed of graphitic carbon, MgO, NiO, and MgCl 2 . Py-GC/MS and TGA-FTIR analyses further demonstrate that the strong oxidative capacity of Ni(III) also promotes deep cleavage and oxidation of aromatic/aliphatic intermediates, which significantly reduces the accumulation of smoke precursors. Moreover, both the Ni(III) and its reduced Ni(II) possess partially filled 3d orbitals capable of scavenging gas-phase radicals (e.g., H· and HO·), thereby interrupting combustion chain reactions and imparting flame-retardant efficacy. Additionally, PDA’s amino/hydroxyl groups strengthen the MOSw-PVC interface via hydrogen bonding, increasing tensile modulus (20.9 MPa) and strength (17.8 MPa) while maintaining impact strength (83.9 kJ/m 2 ). This work establishes a multifunctional design strategy that simultaneously achieves flame retardancy, smoke suppression, and mechanical reinforcement in fPVC composites through synergistic interfacial and catalytic effects.
研究领域:
材料科学
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高分子科学
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化学工程
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纳米技术
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消防安全工程
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表面化学
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分析化学
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物理化学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-14
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IF 16.6
Huang Haoliang,Chang Yu-Chung,Huang Yu-Cheng,Li Lili,Komarek Alexander C.,Tjeng Liu Hao,Orikasa Yuki,Pao Chih-Wen,Chan Ting-Shan,Chen Jin-Ming,Haw Shu-Chih,Zhou Jing,Wang Yifeng,Lin Hong-Ji,Chen Chien-Te,Dong Chung-Li,Kuo Chang-Yang,Wang Jian-Qiang,Hu Zhiwei,Zhang Linjuan
Designing efficient catalyst for the oxygen evolution reaction (OER) is of importance for energy conversion devices. The anionic redox allows formation of O-O bonds and offers higher OER activity than the conventional metal sites. Here, we successfully prepare LiNiO 2 with a dominant 3 d 8 L configuration ( L is a hole at O 2 p ) under high oxygen pressure, and achieve a double ligand holes 3 d 8 L 2 under OER since one electron removal occurs at O 2 p orbitals for Ni III oxides. LiNiO 2 exhibits super-efficient OER activity among LiMO 2 , R MO 3 (M = transition metal, R = rare earth) and other unary 3d catalysts. Multiple in situ/operando spectroscopies reveal Ni III →Ni IV transition together with Li-removal during OER. Our theory indicates that Ni IV (3 d 8 L 2 ) leads to direct O-O coupling between lattice oxygen and *O intermediates accelerating the OER activity. These findings highlight a new way to design the lattice oxygen redox with enough ligand holes created in OER process.
研究领域:
材料科学
·
电化学
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催化
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能源转换
✓ 已验证
DOI
高影响因子
Materials Today Energy
·
2026
·
IF 8.1
Yang Wang,Yiling Feng,Yuxin Zhu,Yizhen Li,Chengjin Chen,Nanjia Yang,Wei Zhu,Zhongbin Zhuang
The electrochemical ethanol oxidation reaction (EOR) in acid offers a promising route for co-producing hydrogen and value-added chemicals, but suffers from severe Pt catalyst poisoning and poor stability. Herein, we report the synthesis of ultrathin PtNi nanowires (NWs) with abundant step defects for efficient and stable EOR. The PtNi NWs/C catalyst exhibits high mass activity (1.50 A mg Pt −1 @0.7 V vs. RHE), Faradaic efficiency (80% to acetic acid), and stability compared to the Pt NWs/C and Pt NPs/C counterparts. It has been demonstrated that the ultrathin NW structure endowed the PtNi NWs/C with high electrochemical active surface area and abundant step sites, while the incorporation of Ni facilitates the removal of poisoning CO and accelerates the EOR kinetics on Pt via the in-situ formation of Ni(III), leading to the superior performance. A practical electrolyzer using the PtNi NW as the anodic catalyst achieves 132 mA cm −2 at 0.8 V and sustains operation for 100 h.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yufei Li,Yuanxiao Duan,Kai Zhang,Wenzheng Yu
Electrocatalytic oxidation of small molecules to replace sluggish water oxidation presents a promising strategy for clean hydrogen production with low energy consumption. Herein, we reported a reliable and universal method to fabricate the leaf-like Co-doped Ni 3 S 2 architecture anchored on Ni mesh. The optimized Co-doped Ni 3 S 2 electrocatalyst exhibits superior electrocatalytic activity toward the alkaline hydrogen evolution reaction (HER) and chemical oxidation as well as excellent durability. Specifically, a significantly reduced cell voltage of 0.80 V is attained at 50 mA cm −2 in sulfion-containing electrolytes, which is about 0.94 and 1.20 V lower than that of urea electrolysis and water splitting, respectively. In situ Raman spectroscopy and electrochemical characterization results imply that the desired oxidation state of the Ni III formed on the surface with shortened oxidation pathway accounts for the increased urea oxidation, whereas a direct electron transfer to surface active sites is responsible for superior sulfion oxidation. In situ spectroscopic evidences further unravel that the sulfion (S 2− ) were stepwisely oxidized to short-chain polysulfides including S 2 2− and S 4 2− and then to elemental sulfur (S 8 ). This work highlights that the integrated overall reaction holds the great promise for saving-energy H 2 generation and environmentally friendly recovery of sulfur with enhanced electron utilization efficiency.
研究领域:
电化学
·
催化
·
材料科学
·
能量转换
·
可持续化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xiaoming Li,Binbin Han,Shuyi Cao,Hongtao Bai,Jingde Li,Xiaohang Du
Efficient bifunctional electrocatalysts towards oxygen evolution reaction (OER) and urea electrooxidation reaction (UOR) are urgently needed for hydrogen production from urea-containing wastewater electrolysis. The main challenge lies in the sluggish UOR kinetics and the stability of catalyst under practical high current density. Here, a vanadium doped heterostructure of Ni(PO 3 ) 2 /Ni 2 P with shaggy nanosheet morphology was successfully synthesized. The doping of V atoms promotes the formation of Ni(PO 3 ) 2 /Ni 2 P heterojunction in phosphating process. It is demonstrated that V-doped Ni(PO 3 ) 2 /Ni 2 P accelerates the generation of real active site V@NiOOH in OER and UOR processes, which can also be stabilized by the PO 3 − ions. The in-situ formed V@NiOOH increases the adsorption energy of urea molecule, and reduces the adsorption energy of key intermediates *COO, thus facilitating the release of CO 2 product from the catalyst surface. The energy barrier of *HNCON to *NCON is also reduced dramatically, promoting the kinetics of UOR. In addition, the shaggy nanosheets morphology provides large number of catalytic sites and transport channels, which are conducive to mass transfer under high current density. As a result, the V-Ni(PO 3 ) 2 /Ni 2 P electrode based anion-exchange membrane (AEM) electrolyzer needs only 1.61 V to drive the total urea electrolysis at an industrial grade current density of 550 mA cm −2 with an outstanding durability of 700 h. This work paves the way for designing practical efficient and stable electrocatalyst for urea contained wastewater electrolysis to produce hydrogen.
研究领域:
材料科学
·
电化学
·
能源转换与存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）