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Highly efficient electrosynthesis of H_(2)O_(2)in acidic electrolyte on metal-free heteroatoms co-doped carbon nanosheets and simultaneously promoting Fenton process

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Chinese Chemical Letters 2024年第7期35卷 514-518页

作者： Xiaodan Wang Yingnan Liu Zhibin Liu Zhongjian Li Tao Zhang Yi Cheng lecheng lei Bin Yang Yang Hou Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310058China Institute of Zhejiang University-Quzhou Quzhou 324000China Donghai Laboratory Zhoushan 316000China Ningbo Institute of Materials Technology&Engineering University of Chinese Academy of SciencesNingbo 315200China School of Biological and Chemical Engineering NingboTech UniversityNingbo 315100China Zhejiang Hengyi Petrochemical Research Institute Co. Ltd.Hangzhou 310058China

Recently electrochemical synthesis of H_(2)O_(2)through oxygen reduction reaction(ORR)via 2e^(-)pathway is considered as a green and on-site ***,it still remains a big challenge for fabricating novel metal-free catalysts under acidic solutions,since it suffers from high overpotential due to the intrinsically week*OOH ***,a co-doped carbon nanosheet(O/N–C)catalyst toward regulating O and N content was synthesized for improving the selectivity and activity of H_(2)O_(2)electrosynthesis *** O/N–C exhibits outstanding 2e-ORR performance with low onset potential of 0.4 V(***)and a selectivity of 92.4%in 0.1 mol/L HClO_(4)*** in situ electrochemical impedance spectroscopy(EIS)tests reveals that the N incorporation contributes to the fast ORR *** density functional theory(DFT)calculations demonstrate that the binding strength of*OOH was optimized by the co-doping of oxygen and nitrogen at certain content,and the O/N–C–COOH site exhibits a lower theoretical overpotential for H_(2)O_(2)formation than O–C–COOH ***,the promoted kinetics for typical organic dye degradation in simultaneous electron-Fenton process on O/N–C catalyst was demonstrated particularly for broadening its environmental application.

关键词： Oxygen reduction Metal-free catalyst H_(2)O_(2)electrosynthesis N doping Carbon materials

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Accelerating Oxygen Electrocatalysis Kinetics on Metal-Organic Frameworks via Bond Length Optimization

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Nano-Micro Letters 2024年第9期16卷 279-290页

作者： Fan He Yingnan Liu Xiaoxuan Yang Yaqi Chen Cheng‑Chieh Yang Chung‑Li Dong Qinggang He Bin Yang Zhongjian Li Yongbo Kuang lecheng lei Liming Dai Yang Hou Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027People’s Republic of China Institute of Zhejiang University-Quzhou Quzhou 324000People’s Republic of China Ningbo Institute of Materials Technology and Engineering Chinese Academy of SciencesNingbo 315201People’s Republic of China School of Biological and Chemical Engineering NingboTech UniversityNingbo 315100People’s Republic of China Department of Physics Tamkang UniversityNew Taipei 25137TaiwanPeople’s Republic of China Australian Carbon Materials Centre(A‑CMC) School of Chemical EngineeringUniversity of New South WalesSydneyNSW 2051Australia

Metal-organic frameworks(MOFs)have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity,but the limited catalytic activity and stability has hampered their practical use in water ***,we develop a bond length adjustment strategy for optimizing naphthalene-based MOFs that synthesized by acid etching Co-naphthalenedicarboxylic acid-based MOFs(donated as AE-CoNDA)to serve as efficient catalyst for water ***-CoNDA exhibits a low overpotential of 260 mV to reach 10 mA cm^(−2)and a small Tafel slope of 62 mV dec^(−1)with excellent stability over 100 *** integrated AE-CoNDA onto BiVO_(4),photocurrent density of 4.3 mA cm^(−2)is achieved at 1.23 *** investigations demonstrate that the stretched Co-O bond length was found to optimize the orbitals hybridization of Co 3d and O 2p,which accounts for the fast kinetics and high *** calculations reveal that the stretched Co-O bond length strengthens the adsorption of oxygen-contained intermediates at the Co active sites for highly efficient water splitting.

关键词： Metal-organic frameworks Bond length adjustment Spin state transition Orbitals hybridization Water splitting

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碳纳米管表面等离子体改性活化过一硫酸盐性能研究

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化学反应工程与工艺 2024年第1期40卷 1-9页

作者：姜涛汪欢雷乐成杨彬浙江大学化学工程与生物工程学院浙江杭州310058 浙江大学衢州研究院浙江衢州324000

将简单高效的等离子体刻蚀方法应用于碳纳米管(CNTs)的表面改性,通过扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线衍射(XRD)、X射线光电子能谱(XPS)和拉曼光谱(Raman)等对改性后的催化剂进行表征分析,结果表明经刻蚀得到的CNTs缺... 详细信息

将简单高效的等离子体刻蚀方法应用于碳纳米管(CNTs)的表面改性,通过扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线衍射(XRD)、X射线光电子能谱(XPS)和拉曼光谱(Raman)等对改性后的催化剂进行表征分析,结果表明经刻蚀得到的CNTs缺陷程度和氧含量均有较大提升。研究发现改性后的CNTs催化剂可有效提升过一硫酸盐(PMS)活化性能,在降解水中2,4-二氯苯酚(2,4-DCP)的性能研究中反应速率为未改性CNTs的3.2倍,30min内2,4-DCP去除率可达到97%,同时在实际水体和放大实验中也展现出良好的性能。淬灭实验和电子顺磁共振实验结果表明体系中主要的活性物质为单线态氧(^(1)O_(2))。本研究提供了一种简单制备高性能非金属活化PMS催化剂的方法,并在水体中有机污染物的去除中展现出良好的应用前景。

关键词：等离子体改性过硫酸盐水处理碳纳米管 2,4-二氯苯酚

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A one-pot process based on P_(44414)Cl-HCl aqueous biphasic system for recovering rare earth elements from NdFeB permanent magnet

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Chinese Chemical Letters 2022年第2期33卷 953-956页

作者： Chuanying Liu Qibin Yan Xingwang Zhang lecheng lei Chengliang Xiao College of Chemical and Biological Engineering Zhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China

Recovering critical metals from secondary resources have attracted great interest *** this work,a green one-pot leaching-extraction process based on tributyl(tetradecyl)phosphonium chloride (P_(44414)Cl)aqueous biphasic system (ABS) was developed to efficiently recover rare earth elements (REEs) from Nd Fe B permanent *** reaction process,phase separation mechanism,and operation conditions were thoroughly *** is found that the P_(44414)Cl-HCl ABS showed strong extraction ability towards Fe (>99%) whereas only a few REEs (<10%) were extracted,leading to extremely high separation selectivity between Fe and *** characterization results showed that the coordination differences of Fe and Nd in HCl were the main driving forces for such highly selective *** phase diagram of P_(44414)Cl-Nd Cl_(3)ABS indicated that the salting-out effect of Nd Cl_(3)was stronger than common *** to the hydrophobic property of P_(44414)[Fe Cl_(4)]and salting-out effect of Nd Cl_(3),the P_(44414)Cl could directly form ABS at room temperature after dissolving practical roasted Nd Fe B samples without any other operations and *** and Fe could be mutually separated in just one *** with traditional liquid-liquid extraction or ABS separation,this recovery process is green and facile and shows great application prospects in the field of rare-earth recovery.

关键词： Rare earth Ionic liquid NdFeB permanent magnet P_(44414)Cl Aqueous biphasic system

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Co anchored on porphyrinic triazine-based frameworks with excellent biocompatibility for conversion of CO_(2)in H_(2)-mediated microbial electrosynthesis

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Frontiers of Chemical Science and Engineering 2022年第12期16卷 1761-1771页

作者： Folin Liu Shaohua Feng Siyuan Xiu Bin Yang Yang Hou lecheng lei Zhongjian Li College of Chemical and Biological Engineering Key Laboratory of Biomass Chemical Engineering of Ministry of EducationZhejiang UniversityHangzhou 310027China Institute of Zhejiang University—Quzhou Quzhou 324000China Academy of Ecological Civilization Zhejiang UniversityHangzhou 310027China

Microbial electrosynthesis is a promising alternative to directly convert CO_(2)into long-chain compounds by coupling inorganic electrocatalysis with biosynthetic ***,problems arose that the conventional electrocatalysts for hydrogen evolution may produce extensive by-products of reactive oxygen species and cause severe metal leaching,both of which induce strong toxicity toward ***,poor stability of electrocatalysts cannot be qualified for long-term *** problems may result in poor biocompatibility between electrocatalysts and *** solve the bottleneck problem,Co anchored on porphyrinic triazine-based frameworks was synthesized as the electrocatalyst for hydrogen evolution and further coupled with Cupriavidus necator *** showed high selectivity for a four-electron pathway of oxygen reduction reaction and low production of reactive oxygen species,owing to the synergistic effect of Co–Nx modulating the charge distribution and adsorption energy of ***,low metal leaching and excellent stability were observed,which may be attributed to low content of Co and the stabilizing effect of ***,the electrocatalyst exhibited excellent ***,the microbial electrosynthesis system equipped with the electrocatalyst successfully converted CO_(2)to poly-β-*** work drew up a novel strategy for enhancing the biocompatibility of electrocatalysts in microbial electrosynthesis system.

关键词： microbial electrosynthesis hydrogen evolution reaction metalloporphyrins biocompatibility CO_(2)conversion

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Spin polarization strategy to deploy proton resource over atomic-level metal sites for highly selective CO_(2) electrolysis

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Frontiers of Chemical Science and Engineering 2022年第12期16卷 1772-1781页

作者： Yingjie Zhao Xinyue Wang Xiahan Sang Sixing Zheng Bin Yang lecheng lei Yang Hou Zhongjian Li Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China Nanostructure Research Centre Wuhan University of TechnologyWuhan 430070China

Unlocking of the extremely inert C=O bond during electrochemical CO_(2) reduction demands subtle regulation on a key“resource”,protons,necessary for intermediate conversion but also readily trapped in water splitting,which is still challenging for developing efficient single-atom catalysts limited by their structural simplicity usually incompetent to handle this *** of extra functional units should be ***,a proton deployment strategy is demonstrated via“atomic and nanostructured iron(A/N-Fe)pairs”,comprising atomically dispersed iron active centers spin-polarized by nanostructured iron carbide ferromagnets,to boost the critical protonation *** as-designed catalyst displays a broad window(300 mV)for CO selectivity>90%(98%maximum),even outperforming numerous cutting-edge M–N–C *** well-placed control of proton dynamics by A/N-Fe can promote*COOH/*CO formation and simultaneously suppress H2 evolution,benefiting from the magnetic-proximity-induced exchange splitting(spin polarization)that properly adjusts energy levels of the Fe sites’d-shells,and further those of the adsorbed intermediates’antibonding molecular orbitals.

关键词： CO_(2)electrolysis/single-atom catalysts/spin polarization/proton dynamics/in situ IR spectroscopy/kinetic isotope effect

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Ultrasmall Pt_(2)Sr alloy nanoparticles as efficient bifunctional electrocatalysts for oxygen reduction and hydrogen evolution in acidic media

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Journal of Energy Chemistry 2022年第1期31卷 315-322,I0009页

作者： Xiangnan Liu Shaoyun Hao Guokui Zheng Zhiwei Su Yahui Wang Qiqi Wang lecheng lei Yi He Xingwang Zhang Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological Engineering Zhejiang UniversityHangzhou 310027ZhejiangChina Institute of Zhejiang University-Quzhou Quzhou 324000ZhejiangChina

Electrocatalytic oxygen reduction reaction(ORR)and hydrogen evolution reaction(HER)in acidic media are vital for the applications of renewable energy ***,the low mass activity of noble Pt urgently needs to be improved due to the strong binding energetics of oxygen species(*O)with Pt *** we report fine PtxSr alloy(-2 nm)supported on N-doped carb on(NC)pyrolyzing from ZIF-8 as bifunctional electrocatalysts toward ORR and HER in acidic *** representative Pt_(2)Sr/NC exhibits an onset potential of 0.94 V *** and half-wave potential of 0.84 V toward ORR,and a low over-potential of 27 mV(10 mA cm^(-2))toward HER,***,the mass activities of Pt_(2)Sr/NC are 6.2 and 2.6 times higher than that of Pt/C toward ORR(at 0.9 V)and HER(at-30 mV),***,Pt_(2)Sr/NC possesses a retention rate of 90.97%toward acidic ORR after 35000 s of continuous *** density functional theory(DFT)calculations and X-ray photoelectron spectroscopy analysis,the incorporation of Sr into Pt forming Pt_(2)Sr alloy redistributes the electronic structures of Pt-Pt bonds,changing the rate-determining step for the ORR on Pt sites from the formation of*OH from*O to the generation of*OOH along with decreasing the energy barrier,which is also confirmed by the downshift of d band ***,the downshift of d band center also leads to the optimization of the adsorption energy(H*)with Pt,significantly improving Pt_(2)Sr/NC toward HER.

关键词： Acidic media Alloy Oxygen reduction reaction Hydrogen evolution reaction Density functional theory

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Rational design on photoelectrodes and devices to boost photoelectrochemical performance of solar-driven water splitting: a mini review

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Frontiers of Chemical Science and Engineering 2022年第6期16卷 777-798页

作者： Siliu Lyu Muhammad Adnan Younis Zhibin Liu Libin Zeng Xianyun Peng Bin Yang Zhongjian Li lecheng lei Yang Hou Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China

As an eco-friendly,efficient,and low-cost technique,photoelectrochemical water splitting has attracted growing interest in the production of clean and sustainable hydrogen by the conversion of abundant solar *** the photoelectrochemical system,the photoelectrode plays a vital role in absorbing the energy of sunlight to trigger the water splitting process and the overall efficiency depends largely on the integration and design of photoelectrochemical *** recent years,the optimization of photoelectrodes and photoelectrochemical devices to achieve highly efficient hydrogen production has been extensively *** this paper,a concise review of recent advances in the modification of nanostructured photoelectrodes and the design of photoelectrochemical devices is ***,the general principles of structural and morphological factors in altering the photoelectrochemical performance of photoelectrodes are ***,the performance indicators and first principles to describe the behaviors of charge carriers are analyzed,which will be of profound guiding significance to increasing the overall efficiency of the photoelectrochemical water splitting ***,current challenges and prospects for an in-depth understanding of reaction mechanisms using advanced characterization technologies and potential strategies for developing novel photoelectrodes and advanced photoelectrochemical water splitting devices are demonstrated.

关键词： photoelectrochemical water splitting photoelectrodes hydrogen production charge separation catalytic mechanism

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Optimizing electronic structure of NiFe LDH with Mn-doping and Fe_(0.64)Ni_(0.36)alloy for alkaline water oxidation under industrial current density

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Nano Research 2023年第7期16卷 8953-8960页

作者： Yang Qian Fan Zhang Lingshu Qiu Weiwei Han Zixu Zeng lecheng lei Yi He Ping Li Xingwang Zhang Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China

Alkaline electrolyzers for water splitting under the industrial current densities are always burdened with huge energy consumption due to the high overpotential and poor stability of the anode nanocatalysts for oxygen evolution reaction(OER).Inspired by the interfacial charge transfer for enhancing the performance,a series of in-situ grown interfacial Mn-NiFe lactate dehydrogenase(LDH)was designed on the Fe_(0.64)Ni_(0.36)/NM(nickel mesh)alloy *** optimized Mn_(0.15)-NiFe LDH/Fe_(0.64)Ni_(0.36)/NM exhibited an ultralow overpotential of 295 mV to drive 500 mA·cm^(-2)and an incredible stability under large current *** interfacial space and heteroatom doping synergistically triggered the electronic structure optimization to promote electron transfer and ensure the durability of the high-current ***,the designed Mn_(0.15)-NiFe LDH/Fe_(0.64)Ni_(0.36)/NM as an anode in an integral alkaline electrolyzer exhibited a cell voltage of 1.78 V at 500 mA·cm^(-2) with a stability of 366 *** functional theory(DFT)calculations further demonstrated the synergistic effect of alloy layer introduction and Mn doping could accelerate electron transfer and stabilize the charged active center to activate the NiFe LDH and reduce the OER energy *** work offers new insights into developing efficient self-supported catalysts for high-current alkaline water oxidation.

关键词： heteroatom doping alloy layer introduction synergistic effect high-current alkaline water oxidation

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Layered bismuth oxide/bismuth sulfide supported on carrageenan derived carbon for efficient carbon dioxide electroreduction to formate

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Chinese Journal of Chemical Engineering 2022年第3期35卷 116-123页

作者： Xiangzhao Hu Junjie Sun Wanzhen Zheng Sixing Zheng Yu Xie Xiang Gao Bin Yang Zhongjian Li lecheng lei Yang Hou Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China Department of Material Chemistry Nanchang Hangkong UniversityNanchang 330063China School of Biological and Chemical Engineering Ningbo Technology UniversityNingbo 315100China

Electrochemical reduction of carbon dioxide(CO_(2)ER)into formate plays a crucial role in CO_(2)conversion and ***,it still faces the problems of high overpotential and poor catalytic ***,we report a hybrid CO_(2)ER electrocatalyst composed of layered bismuth sulfide(Bi_(2)S_(3))and bismuth oxide(Bi_(2)O_(3))supported on carrageenan derived carbon(Bi-CDC)prepared by a combined pyrolysis with hydrothermal *** such 3 D hybrid,layered Bi_(2)O_(3)and Bi_(2)S_(3)are uniformly grown on nanocarbon *** from strong synergistic effect between Bi_(2)O_(3)/Bi_(2)S_(3)and nanocarbon,Bi-CDC-1:2 displays a high Faradic efficiency(FE)of>80%for formate production in the range of-0.9 V to-1.1 V with the maximum formate FE of 85.6%and current density of 14.1 mA·cm^(-2) at-1.0 ***,a positive onset potential of-0.5 V,a low Tafel slope of 112.38 mV·dec^(-1),and a slight performance loss during long-term CO_(2)ER tests are observed on Bi-CDC-1:*** results shows that the better CO_(2)ER performance of Bi-CDC-1:2 than that of Bi_(2)O_(3)can be attributed to the strong interfacial interactions between nanocarbons and Bi_(2)O_(3)/Bi_(2)S_(3).In situ ATR-FTIR measurements reveal that the rate-determining step in the CO_(2)ER is the formation of HCOO^(*) *** with carbon support,Bi-CDC-1:2 can promote the production of HCOO^(*) intermediate and thus promoting CO_(2)ER kinetic.

关键词： Nanomaterials Catalyst Selectivity Bi_(2)S_(3)/Bi_(2)O_(3) CO_(2)electroreduction Formate

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