Science China-Materials
·
2025
·
IF 7.4
Yu Jianli,Shen Yongli,Zhu Pei,Li Lina,An Changhua
Sluggish water dissociation kinetics in the alkaline hydrogen evolution reaction (HER) continue to hamper its practical production. Herein, a class of heterojunction electrocatalyst featuring Ru-Ni(OH) 2 interfaces on nickel foam (NF) with self-engineered built-in electric fields (BIEF) has been synthesized via a simple in situ galvanic replacement reaction. The as-made hierarchical architecture of Ru-Ni (OH) 2 /NF exhibits a record overpotential of 9.6 mV at a current density of 10 mA cm −2 for alkaline HER, surpassing most reported catalysts and the commercial Pt/C benchmark. Furthermore, it also reveals exceptional catalytic activity towards hydrazine oxidation reaction (HzOR) at 100 mA cm −2 with a remarkably low potential of ca. 0.015 V vs. RHE (reversible hydrogen electrode). The assembled overall hydrazine splitting (OHzS) system integrating HER and HzOR requires a cell voltage of about 0.09 V to reach 50 mA cm −2 , which is 1.637 V lower than the corresponding overall water splitting (OWS) device. Systematic analysis and calculation reveal that the BIEF induces the redistribution of interfacial electrons for Ru, facilitating H 2 O dissociation and intermediates conversion to deliver the ultra-high electrocatalytic performance. This work provides an avenue for the design and preparation of electric field-mediated catalysts towards sustainable energy conversion.
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高影响因子
DALTON TRANSACTIONS
·
2021
·Vol. 51
·期 5
·1979-1984
·
IF 4.39
Huaiyu Hu,Junben Huang,Zhiyong Guo,Min Zhang,Zhihua Yang,Shilie Pan
The first alkaline earth metal borate-nitrate, namely Ba2B5O8(OH)2(NO3)·3H2O (BBNOH), has been synthesized by the hydrothermal method. BBNOH crystallizes in the space group of P21/c and shows two-dimensional (2D) 2∞[B5O8(OH)2]3− borate anion layers, and the hydrated barium cations and the [NO3]− anions are located between the layers. The process of optimizing the structure of Ba2B5O8(OH)2OH to BBNOH has been discussed. The first principles calculation has been used to calculate the birefringence of Ba2B5O8(OH)2(NO3)·3H2O, and the value is 0.033@1064 nm, which is mainly originated from the borate anions and the π conjugated [NO3]− anions.
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Science China-Chemistry
·
2026
·
IF 9.7
Zheng Xia,Fu Yaoqiang,Ning Jing,Wang Haorui,Liu Hongfei,Cui Chunhua
Direct formate fuel cells (DFFCs) are becoming one of the most promising next-generation energy devices owing to their high energy density, low toxicity, and carbon neutrality. However, their practical application is hindered by the sluggish kinetics of the formate oxidation reaction (FOR) on conventional palladium (Pd)-based catalysts due to the strong adsorption of hydrogen intermediates (H ads ) that block the active sites. Herein, we tackled the above problem by tailoring the Pd electrocatalytic properties through the interfacial interaction with the hydroxyl group-abundant and oxophilic Co(OH) 2 substrate. This resulted in an impressive mass activity of 5.02 A mg
−1 Pd
for the synthesized Pd/Co(OH) 2 , approximately three times that of commercial Pd/C. Moreover, under high formate concentration, Pd/Co(OH) 2 exhibits significantly improved stability, i.e. , up to 24000 s sustainable current density with 100% selectivity toward CO 2 (CO 2 is actually converted to carbonate in alkaline media). Kinetic isotope effect (KIE) analysis and in situ Raman spectroscopy based mechanistic study reveal the excellent FOR performance of Pd/Co(OH) 2 originates from the partially oxidized Pd facilitated H ads oxidative removal and the more hydrophilic surface induced competitive HCOO − adsorption over H ads . This study demonstrates a rational strategy to optimize the Pd-based FOR electrocatalysts through the electronic and interfacial interactions with appropriate substrate to modulate the key intermediate adsorption-reaction kinetics.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122309
·
IF 7.5
Hongjiang Peng,Yanyu Song,Cong Lu,Gongjie Hua,Jinhong Wu,Kuangfei Lin
Advanced oxidation processes based on peroxymonosulfate (PMS) activation show promising application prospects in the field of water treatment, yet the efficient utilization of reactive oxygen species (ROS) in different spatial regions (bulk solution and catalyst surface) remains challenging. In this work, a catalyst consisting of trace cobalt ion-complexed hydroxyapatite (Co-HAP) was prepared, which exhibits excellent spatial synergistic oxidation effects. Bulk SO 4 •− and in-situ generated surface •OH ensure the efficient removal of levofloxacin (LEV) (74.5% within 20 min). Quenching experiments reveal the surface-mediated ROS evolution pathway, where bulk SO 4 •− reacts with the abundant lattice hydroxyl groups (-OH) on the HAP surface to in-situ generate surface-bound hydroxyl radicals (•OH surf ). Bulk SO 4 •− originates from the activation of PMS by Co ions. Electrochemical characterization and charge density difference simulation confirm that PMS receives electrons from the catalyst, thus inducing the breakage of O-O bonds to generate SO 4 •− . Therefore, bulk SO 4 •− is responsible for attacking dissolved pollutants, while LEV adsorbed on the catalyst surface is "precisely targeted" by surface-confined •OH. This "two-pronged" synergistic strategy significantly reduces mass transfer resistance and achieves efficient utilization of ROS, thereby the degradation rate ( k obs value) of LEV by Co-HAP is 4.6 times that by Co ions alone. Moreover, the Co-HAP system exhibits excellent stability and promising anti-interference ability. This study provides new insights into the positive role of carrier surface functional groups in regulating ROS distribution and evolution in heterogeneous catalysis.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Xiaohui Chen,Zhishuncheng Li,Zhishan Li,Jia Liu,Zhouhang Li,Hua Wang,Kongzhai Li
Hydrogen energy represents a promising, sustainable and clean energy resource. However, widespread application of water electrolysis for hydrogen production remains limited by the reliance on expensive noble-metal-based catalysts. Developing cost-effective and efficient electrocatalysts is therefore crucial. Herein, we propose a novel heterostructure strategy to prepare non-noble-metal-based catalysts for overall water splitting. Through a simple two-step synthesis, NiTe-supported catalysts were fabricated: NF/NiTe/NiFe(OH) x -2 for the oxygen evolution reaction (OER) and NF/NiTe/Pt for the hydrogen evolution reaction (HER). Electrochemical measurements revealed outstanding catalytic activities: the optimized catalysts achieved current densities of 10 mA cm −2 at low overpotentials of 264 mV for the OER and 30 mV for the HER. When integrated into a two-electrode electrolyzer, the system required only 1.55 V to reach 10 mA cm −2 and 1.73 V to reach 100 mA cm −2 , while maintaining stable operation for 100 h and 50 h, respectively. Density functional theory calculations reveal that the Pt/NiTe heterostructure possesses a near-optimal Gibbs free energy for hydrogen adsorption (ΔG H* =-0.06 eV), which substantially accelerates HER kinetics. This work provides fundamental insights into heterostructure design and offers guidance for the rational development of efficient nanomaterials for catalytic applications.
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Nature Communications
·
2026
·
IF 18.1
Mao Qiqi,Wang Wenxin,Yang Ruidong,Deng Kai,Yu Hongjie,Li Wenzhen,Wang Liang,Wang Hongjing,Guo Shaojun
Industrial-level alkynols electrocatalytic semi-hydrogenation using seawater as hydrogen source offers a sustainable alternative to conventional thermocatalytic routes, yet remains limited by the lack of efficient and robust electrocatalysts. Here, we report the synthesis of Nd 1 Gd 1 dual atomic site on metallene for co-production of alkenol and magnesium hydroxide in the seawater system. Nd 1 Gd 1 Pd metallene achieves a selectivity of ≈96.7% and a Faradaic efficiency of ≈87.3% for the conversion of 2-methyl-3-butyn-2-ol to 2-methyl-3-buten-2-ol at −150 mA cm -2 in a flow-cell system, and maintains ≈98.0% selectivity at 1.2 A for over 300 h of continuous operation, achieving the long-term stable co-electrosynthesis of alkenols and magnesium hydroxide in natural seawater at industrial-scale currents. Techno-economic analysis reveals a projected product revenue of at least $8,499 per ton of 2-methyl-3-buten-2-ol, underlining the industrial viability of this process. Mechanism investigations illustrate dual hydrogen-spillover and co-catalytic effects on Nd 1 Gd 1 Pd, promoting migration-reaction coupling mechanism of reactive *H to synergize hydrogenation. This work provides a seawater electrocatalytic semi-hydrogenation system and proposes an optimization strategy by atomically engineered dual hydrogen-spillover effect.
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高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122633
·
IF 7.5
Xiaoxuan Li,Ying Lv,Jiaxin Du,Xuelian Chen,Meixia Xiao,Shubin Lei
Defect engineering coupled with heterojunction construction represents a pivotal strategy for optimizing the charge separation dynamics of photocatalysts. Herein, we report the fabrication of a novel Z-scheme heterojunction composed of bismuth-based metal-organic frameworks (NOTT-220) and layered Bi 2 O 2 [BO 2 (OH)] nanosheets via a hydrothermal approach. To further potentiate the photocatalytic activity, surface oxygen vacancies (OVs) were precisely introduced into the heterostructure through controlled ultraviolet (UV) irradiation. This defect-rich engineering strategy significantly broadened the visible-light absorption range and facilitated the separation of photogenerated carriers. Consequently, the optimized catalyst (OVs-BN-20) exhibited a superior photocatalytic reaction rate constant of 0.8133 min −1 , achieving 95.9% degradation rate of CIP within 2 h. Detailed mechanistic investigations, including liquid chromatography-mass spectrometry (LC-MS) and electron spin resonance (ESR), elucidated the degradation pathways and confirmed the synergistic role of superoxide radicals (·O 2 -) and photogenerated holes (h + ). This work not only provides a facile pathway for designing defect-modulated Z-scheme photocatalysts but also offers profound insights into the mineralization mechanisms of persistent antibiotic pollutants.
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Journal of Cleaner Production
·
2023
·
IF 11.1
Yicong Wang,Sisuo Zhang,Richard L. Smith,Xiaoning Liu,Xinhua Qi
Effective removal of both nitrogen and phosphorus from water is of great importance for maintaining the safety of the environment. In this work, ordered mesoporous carbon electrode materials containing La(OH) 3 and Fe 3 C components (La#OMC-Fe 3 C) were prepared by combining solvent evaporation induced self-assembly and impregnation methods. The ordered pores in La#OMC-Fe 3 C facilitated electron transfer at the electrode-solution interface during nitrate reduction and provided voids for phosphate removal . In the electrochemical system, Fe 3 C in the electrode supplied electrons for nitrate reduction and gave the electrode a high degree of stability, whereas La(OH) 3 selectively removed phosphate, thus avoiding byproduct precipitation from solution. The electrode material maintained efficient electrochemical nitrogen and phosphorus removal over a wide range of conditions including pH (3–11) and aqueous environments containing multiple ions (Cl − , SO 4 2− , K + , Na + , Ca 2+ , Mg 2+ ) or actual aqueous environments (seawater). After 10 cycles, the performance of La#OMC-Fe 3 C for nitrogen and phosphorus removal remained above 97%. This work realizes the simultaneous removal of nitrogen and phosphorus in the electrochemical system, and solves the problems of precipitation in water and non-circulation of electrodes, which can provide a new strategy for the treatment of eutrophic water in practical production.
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Nanomaterials
·
2023
·Vol. 13
·期 3
·493
·
IF 5.3
Meng Shao,Jun Li,Jing Li,Yanan Yan,Ruoliu Li
Honeycomb-like Ni(OH)2/Ni3S2/Ni foam (NF) was fabricated via a two-step hydrothermal process and subsequent alkalization. Ni3S2with a honeycombed structure was in-situ synthesized on the NF surface by a hydrothermal process. MOF-derived Ni(OH)2nanosheets were then successfully grown on the Ni3S2/NF surface by a second hydrothermal process and alkaline treatment, and a large number of nanosheets were interconnected to form a typical honeycomb-like structure with a large specific surface area and porosity. As a binder-free electrode, the prepared honeycomb-like Ni(OH)2/Ni3S2/NF exhibited a high specific capacitance (2207 F·g−1at 1 A·g−1, 1929.7 F·g−1at 5 mV·s−1) and a remarkable rate capability and cycling stability, with 62.3% of the initial value (1 A·g−1) retained at 10 A·g−1and 90.4% of the initial value (first circle at 50 mV·s−1) retained after 5000 cycles. A hybrid supercapacitor (HSC) was assembled with Ni(OH)2/Ni3S2/NF as the positive electrode and activated carbon (AC) as the negative electrode and exhibited an outstanding energy density of 24.5 Wh·kg−1at the power density of 375 W·kg−1. These encouraging results render the electrode a potential candidate for energy storage.Keywords:Ni(OH)2/Ni3S2/NF;honeycomb-like structure;two-step hydrothermal;alkalization;MOF-derived Ni(OH)2;supercapacitor
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高影响因子
TALANTA
·
2023
·
IF 6.1
Xiaojun Wen,Huan Cheng,Weilong Zhang,Lijun You,Jumei Li
To enable the widespread application of surface-enhanced Raman scattering (SERS) technique in practical sensing of organic pollutants, it is essential to develop a reliable SERS substrate that offers both high sensitivity and reusability. In this study, we employed a simple and rapid in-situ deposition method to coat Ag nanoparticles onto flower-like Ni(OH) 2 spheres, resulting in the formation of Ni(OH) 2 /Ag composites with excellent photocatalytic performance and SERS activity. These composites were used as a promising SERS analysis tool for effective detection of organic pollutants, including ciprofloxacin hydrochloride (CIP) and methylene blue (MB). Notably, the composites exhibited outstanding detection limits of 10 −8 M for MB and 10 −7 M for CIP, respectively, and showed a strong linear relationship between SERS intensities and the logarithmic concentration (R 2 ≥ 0.97). Moreover, under simulated sunlight irradiation, the Ni(OH) 2 /Ag composites efficiently degraded MB and CIP molecules within a short period of 120 min for MB and 130 min for CIP. This demonstrated their practical reusability, as evidenced by their consistent performance over five cycles of SERS sensing. These findings underscore the significant potential of these composites for SERS-based detection of trace pollutants and ecological restoration through photocatalytic reactions in the future.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Chao Qu,Yan-gang Li,Shu-juan Meng,Xiao-hu Li,Shu-jun Zhang,Da-wei Liang
Recently, carbon nanotubes coated carbon black and polytetrafluoroethylene (CNTs-C/PTFE) gas diffusion electrode was used as an air-cathode in an electro-oxidation (EO) system for effectively generating hydrogen peroxide (H 2 O 2 ) through a 2-electron oxygen reduction reaction (ORR). This ORR-EO system not only lowered applied voltage and conserved energy, but the synergistic peroxone (O 3 /H 2 O 2 ) reaction could increase hydroxyl radicals ( • OH) generation for organics elimination. However, a significant proportion of H 2 O 2 was left in the effluent of ORR-EO, which was a loss of resources and energy. In this study, a Fenton-like reaction for in-situ H 2 O 2 decomposition to generate active oxidation species was inserted by introducing MnO 2 into the cathodic catalyst layer, and the sole MnO 2 /CNTs-C/PTFE air-cathode could accomplish 90% of phenol degradation. When MnO 2 /CNTs-C/PTFE air-cathode combined with Ti/NATO anode in an ORR-EO system, all anodic oxidation, Fenton-like reaction, and peroxone took place to successfully generate • OH and singlet oxygen ( 1 O 2 ). Over 95% of TOC in phenol and landfill leachate bio-effluent was effectively eliminated, with 20% energy savings compared to the ORR-EO with CNTs-C/PTFE air cathode.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Hao Wang,Hongyou Yin,Zeng Zhang,Yan Wu,Chang Yi,Tingting Shen
γ-Cu 2 (OH) 3 Cl is used as a Fenton catalyst to mineralize phenol in high chloride solutions. The mineralization of phenol can be enhanced even at 15000 mg∙L –1 NaCl under ambient pH. In addition, other aromatic contaminants including bisphenol A , benzoic acid , 2-chlorophenol, salicylic acid and aniline can also be effectively mineralized under the high chloride concentration. However, reference catalysts including CuSO 4 , CuO and Cu 2 O are significantly depressed by chloride. The chloride resistance ability of γ-Cu 2 (OH) 3 Cl is proposed. First, σ-Cu-ligand complexes formed between Cu 2+ and phenolic hydroxyl can react with H 2 O 2 to promote the rapid reduction of Cu 2+ to Cu + , which are not hindered by chloride. Second, the self-redox property of γ-Cu 2 (OH) 3 Cl which initiates the electron transfer from H 2 O 2 to Cu 2+ to generate Cu + is improved by chloride. Third, the circumneutral pH could suppress HO• scavenging by chloride. The activation energies of phenol mineralization over γ-Cu 2 (OH) 3 Cl in chloride-free and high chloride solutions are 42.9 and 32.3 kJ∙mol –1 , respectively. Chloride does not change the phenol mineralization pathway but accelerates its degradation into small carboxylic acids.
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