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Efficient removal of natural organo-chromium(Ⅲ)through selfcirculating decomplex and immobilization with nanoscale zerovalent iron

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Nano research 2024年第1期17卷 364-371页

作者： Zhicheng Dong Yunyun Xu Can Wu Jin Chao Chen Tian Zhang Lin School of metallurgy and Environment Central South UniversityChangsha 410083China chinese national engineering research center for control&treatment of heavy metal pollution Changsha 410083China College of Ecology and Environment Chengdu University of TechnologyChengdu 610059China School of Environment and energy The Key Laboratory of Pollution Control and Ecosystem Restoration in Industry Clusters(Ministry of Education)South China University of TechnologyGuangzhou 510006China

Organo-chromium(III)complex is one of the chromium contaminant species,which would transform to high-toxic Cr(VI)during migrating in the *** natural organo-chromium(III)(NOCr)is difficult to remove by traditional degradation or precipitation methods,due to its high stability and ***,we demonstrated a novel NOCr removing method by transforming it to certain structures similar to Cr-Fe minerals in nature,through a self-circulating decomplex and immobilization mechanism with nano zero-valent iron(nZVI).Taking chromium glycinate(Cr-Gly)as a probe,nZVI showed a high Cr removal efficiency of 99.4%under ambient *** removal process included three stages of adsorption,decomplexation,and ***-Gly was first adsorbed on the surface of nZVI by chemisorption of the oxide ***,the adsorbed Cr-Gly was decomplexed and oxidized to Cr(VI)by·OH and 1O_(2),which were generated from molecular oxygen activated by ***,the released Cr(VI)could be in-situ adsorbed and re-reduced to Cr(III),which was further immobilized in form of Cr-O-Fe *** the Cr-O-Fe complexing structure was similar to that of Cr-Fe minerals(such as chromohercynite)in nature,this work explored a novel and efficient NOCr removing method that was potential to weaken chromium pollution in the environment.

关键词： organo-chromium(III) zero-valent iron adsorption decomplexation Cr immobilization

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Atomically Dispersed Zinc Active Sites Efficiently Promote the Electrochemical Conversion of N2 to NH3

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energy & Environmental Materials 2024年第3期7卷 179-185页

作者： Yanjiao Wei Xinyu Wang Mengjie Sun Min Ma Jian Tian Minhua Shao School of Materials Science and engineering Shandong University of Science and Technology Department of Chemical and Biological engineering The Hong Kong University of Science and Technology energy institute and Chinese National Engineering Research Center for Control & Treatment of Heavy Metal PollutionThe Hong Kong University of Science and Technology

At present,the research on highly active and stable nitrogen reduction reaction catalysts is still challenging work for the electrosynthesis of ammonia （NH3）.Herein,we synthesized atomically dispersed zinc active sites supported on N-doped carbon nanosheets （Zn/NC NSs） as an efficient nitrogen reduction reaction catalyst,which achieves a high ammonia yield of46.62μ***-0.85 V （vs RHE） and Faradaic efficiency of 95.8%at-0.70 V （vs RHE）.In addition,Zn/NC NSs present great stability and selectivity,and there is no significant change in NH3rate and Faradaic efficiencies after multiple *** structural characterization shows that the active center in the nitrogen reduction reaction process is the Zn-N4sites in the *** calculation confirms that Zn/NC with Zn-N4configuration has a lower energy barrier for the formation of*NNH intermediate compared with pure N-doped carbon nanosheets （N-C NSs）,thus promoting the hydrogenation kinetics in the whole nitrogen reduction reaction process.

关键词： electrocatalysis nitrogen reduction single-atom catalyst Zn–N4

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Highly active and durable core-shell electrocatalysts for proton exchange membrane fuel cells

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Nano research 2024年第10期17卷 8772-8784页

作者： Hsiwen Wu Fei Xiao Jing Wang Meng Gu Minhua Shao Department of Chemical and Biological engineering The Hong Kong University of Science and TechnologyClear Water BayHong KongChina Department of Materials Science and engineering Southern University of Science and TechnologyShenzhen 518055China Fok Ying Tung research institute The Hong Kong University of Science and TechnologyGuangzhou 511458China energy institute and chinese national engineering research center for control&treatment of heavy metal pollution The Hong Kong University of Science and TechnologyClear Water BayHong KongChina

This work presents simple post-treatment methods to selectively and partially remove the Pd core of Pd-Pt core–shell(Pt@Pd/C)*** proton exchange membrane fuel cell with the post-treated Pt@Pd/C cathode(Pt loading:0.10 mg·cm^(-2))delivers an impressive peak power density of 1.2 W·cm^(-2).The partial removal of Pd core endows an ultrahigh oxygen reduction reaction(ORR)mass activity of 0.32 A·g_(PGM)-1 when normalized to the platinum group metal(PGM)mass,or equivalently 0.55 A·mg_(Pt)^(-1) at 0.9 V measured in a fuel *** post-treatment thickens the Pt shells and mitigates the Pd dissolution during potential *** a result,the post-treated core-shell catalyst demonstrates superior durability in ORR mass activity and polarization power density retention than untreated core-shell catalyst and benchmark Pt/***-situ inductively coupled plasmamass spectrometry(ICP-MS)results highlight that the amount of dissolved Pd in post-treated core–shell catalyst is 17-times lower than that of the untreated *** findings highlight the importance of structural tuning of catalysts in enhancing their mass activity and durability.

关键词： core-shell catalyst platinum monolayer proton exchange membrane fuel cell oxygen reduction reaction durability

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Preparation of Fe-As alloys by mechanical alloying and vacuum hot-pressed sintering:microstructure evolution,mechanical properties,and mechanisms

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Rare metals 2024年第8期43卷 3876-3892页

作者： Fei Chai Fei-Ping Zhao Zhan Hu Shi-Yi Wen Ben-Hammouda Samia Ze-Lin Fu Xin-Ting Lai Yan-Jie Liang Xiao-Bo Min Li-Yuan Chai School of metallurgy and Environment Central South UniversityChangsha 410083China chinese national engineering research center for control&treatment of heavy metal pollution Institute of Environmental EngineeringCentral South UniversityChangsha 410083HunanChin State Key Laboratory of Powder metallurgy Central South UniversityChangsha 410083China Department of Building Civiland Environmental EngineeringConcordia UniversityMontreal H3G 1M8Canada

Arsenic materials have attracted great attention due to their unique ***,research concerning iron-arsenic(Fe-As) alloys is very scarce due to the volatility of As at low temperature and the high melting point of ***,a new Fe-As alloy was obtained by mechanical alloying(MA) followed by vacuum hot-pressed sintering(VHPS).Moreover,a systematic study was carried out on the microstructural evolution,phase composition,leaching toxicity of As,and physical and mechanical properties of Fe-As alloys with varying weight fractions of As(20%,25%,30%,35%,45%,55%,65%,and 75%).The results showed that pre-alloyed metallic powders(PAMPs) have a fine grain size and specific supersaturated solid solution after MA,which could effectively improve the mechanical properties of Fe-As alloys by VHPS.A high density(> 7.350 g·cm^(-3)),low toxicity,and excellent mechanical properties could be obtained for FeAs alloys sintered via VHPS by adding an appropriate amount of As,which is more valuable than commercial Fe-As *** Fe-25% As alloy with low toxicity and a relatively high density(7.635 g·cm^(-3)) provides an ultra-high compressive strength(1989.19 MPa),while the Fe-65% As alloy owns the maximum Vickers hardness(HVo.5 899.41).After leaching by the toxicity characteristic leaching procedure(TCLP),these alloys could still maintain good mechanical performance,and the strengthening mechanisms of Fe-As alloys before and after leaching were *** in the grain size,micro structure,and phase distribution induced significant differences in the compressive strength and hardness.

关键词： Mechanical alloying Vacuum hot-pressed sintering High-pressure Arsenic-iron alloys Mechanical properties

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Efficient C-N coupling in electrocatalytic urea generation on copper carbonate hydroxide electrocatalysts

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Journal of energy Chemistry 2024年第6期93卷 289-298,I0008页

作者： Yinuo Wang Yian Wang Qinglan Zhao Hongming Xu Shangqian Zhu Fei Yang Ernest P.Delmo Xiaoyi Qiu Chi Song Juhee Jang Tiehuai Li Ping Gao MDanny Gu Minhua Shao Advanced Materials Thrust The Hong Kong University of Science and Technology(Guangzhou)Guangzhou 511400GuangdongChina Department of Chemical and Biological engineering The Hong Kong University of Science and TechnologyClear Water BayKowloonHong KongChina Department of Materials Science and engineering Southern University of Science and Technology of Chin11088 Xueyuan BoulevardShenzhen 518055GuangdongChina energy institute and Chinese National Engineering Research Center for Control&Treatment of Heavy Metal PollutionThe Hong Kong University of Science and TechnologyKowloonHong KongChina Department of Chemistry City University of Hong KongTat Chee AvenueKowloonHong KongChina

Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of ***,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen *** thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~**** work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.

关键词： Copper carbonate hydroxide Co-reduction Urea generation C-N coupling DFT calculation

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Solid Bronsted acidity boosts adsorption reactivity of nano-adsorbent for water decontamination

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Frontiers of Environmental Science & engineering 2024年第7期18卷 23-34页

作者： Sikai Cheng Zhixian Li Kaisheng Zhang Qingrui Zhang Xiaolin Zhang Bingcai Pan State Key Laboratory of pollution control and Resource Reuse School of the EnvironmentNanjing UniversityNanjing 210023China Environmental Materials and pollution control Laboratory Institute of Solid State PhysicsHFIPSChinese Academy of SciencesHefei 230031China State Key Laboratory of Metastable Materials Science and Technology Yanshan UniversityQinhuangdao 066004China Hebei Key Laboratory of heavy metal Deep-remediation in Water and Resource Reused Qinhuangdao 066004China research center for Environmental Nanotechnology(ReCENT) Nanjing UniversityNanjing 210023China

Despite the development of various Lewis acidic nano-adsorbents for fluoride removal through innersphere coordination,strong competition for hydroxyl ions still hinders efficient water *** addition,the critical issue of polysilicate scaling that results from the ubiquitous silicates must be *** tackle these issues,an alternative approach to enhancing adsorption reactivity by modifying nano-adsorbents with dual Lewis and Bronsted acidity is *** feasibility of this approach is demonstrated by growing zirconium phosphate(ZrP)inside a gel-type anion exchanger,N201,to produce nanocomposite ZrP@N201,in which the confined ZrP contained an otherwise metastable amorphous phase with Lewis acidic Zr^(4+) sites and Bronsted acidic monohydrogen phosphate groups(-O_(3)POH).Compared with the Lewis acidic nano-zirconium oxide analog(HZ0@N201),ZrP@N201 exhibited a greatly improved adsorption capacity(117.9 vs.52.3 mg/g-Zr)and mass transfer rate(3.56×10^(-6) vs.4.55×10^(-7) cm/s),while bulk ZrP produced a thermodynamically stableα-phase with Bronsted acidity that exhibited negligible adsorption capability toward *** enhanced defluoridation activity of ZrP@N201 is attributed to Bronsted acidity and the increased outer electron density of ZA+sites,as corroborated using XPS and solid-state NMR ***,Bronsted acidity strengthens the resistance of ZrP@N201 to silicate,allowing its full regeneration during cyclic *** tests demonstrated 3-10 times the amount of clean water from(waste)for ZrP@N201 as compared to both HZO@N201 and the widely used activated aluminum *** study highlights the potential of developing nano-adsorbents with dual acidities for various environmental remediation applications.

关键词： Nanocomposite Selective adsorption Fluoride removal Dual Lewis and Bronsted acidity Regeneration

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Recovery of cathode copper and ternary precursors from CuS slag derived by waste lithium-ion batteries:Process analysis and evaluation

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chinese Chemical Letters 2024年第7期35卷 178-182页

作者： Yun Wei Lei Zhou Wenbin Hu Liming Yang Guang Yang Chaoqiang Wang Hui Shi Fei Han Yufa Feng Xuan Ding Penghui Shao Xubiao Luo national-Local Joint engineering research center of heavy metals Pollutants control and Resource Utilization Nanchang Hangkong UniversityNanchang 330063China School of Life Science Jinggangshan UniversityJi’an 343009China CAS Key Laboratory of Green Process and engineering National Engineering Research Center of Green Recycling for Strategic Metal ResourcesInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China Biomass Molecular engineering center and Anhui Provincial Key Laboratory of Microbial Pest control Anhui Agricultural UniversityHefei 230036China Jiangxi Ganfeng Recycling Technology Co.LTD. Xinyu 338004China

The efficient and environmentally friendly recycling technology of waste residue that including abundant heavy metal produced during the recovery of lithium batteries has become a research ***,a novelty process of acid leaching-selective electrodeposition-deep impurity removal-regeneration was proposed to recovery of the CuS slag,which has been efficient transferred to high purity cathode copper and commercially available ternary *** cathode with a purity of 99.67%was prepared under electrochemical reaction conditions at-0.55 V for 2 h.A novel impurity remover-Mn powder,which was used to remove the residual impurities and as a feedstock for the ternary ***,NCM523 was regenerated by *** process is superior to the traditional process in economy,energy consumption,CO_(2)emissions,product purity and process *** study provides a new approach for solid waste recovery and precious metal enrichment.

关键词： CuS slag Electrodeposition Cathode copper Ternary precursor Solid waste recovery

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海胆状CoTe-CoP异质结构催化剂在全pH范围内高效析氢

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Science China Materials 2024年第6期67卷 1891-1899页

作者：朱少柯邢明辉路站宽乔泽龙王世涛赵青蓝邵敏华甑崇礼曹达鹏 State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China Department of Chemical and Biological engineering Hong Kong University of Science and TechnologyClear Water BayKowloonHong Kong 999077China energy institute and Chinese National Engineering Research Center for Control&Treatment of Heavy Metal PollutionThe Hong Kong University of Science and TechnologyClear Water BayKowloonHong Kong 999077China Qingdao International Academician Park research institute Qingdao 266000China School of Chemical engineering The University of New South WalesSydney NSW 2052Australia

研发长效稳定、pH适应性强的析氢反应(HER)催化剂对实现大规模制氢具有重要意义.界面工程是研发高效HER催化剂的有效策略之一.本文成功构建了海胆状异质结构催化剂CoTe-CoP/***和CoP的协同作用不仅优化了电子结构、暴露了更多的活性位点... 详细信息

研发长效稳定、pH适应性强的析氢反应(HER)催化剂对实现大规模制氢具有重要意义.界面工程是研发高效HER催化剂的有效策略之一.本文成功构建了海胆状异质结构催化剂CoTe-CoP/***和CoP的协同作用不仅优化了电子结构、暴露了更多的活性位点,而且有效地提高了催化剂的亲水性和疏气性.密度泛函理论计算表明:CoTe与CoP之间的相互作用有效地降低了水的解离能垒,同时增强了对H~*的吸附.这些结果使得CoTe-CoP/NF在整个pH范围内具有优异的HER性能和催化稳定性.在酸性、碱性和中性介质中,CoTe-CoP/NF电极驱动10 mA cm^(-2)的电流密度仅需51、53和75 mV的过电位.总之,本工作为在全pH范围内构建高性能HER催化剂提供了一种界面工程新策略.

关键词： heterostructure hydrogen evolution reactions in-terface engineering all-pH range synergy effect

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High-silica faujasite zeolite-tailored metal encapsulation for the low-temperature production of pentanoic biofuels

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Journal of energy Chemistry 2024年第1期88卷 552-560,I0012页

作者： Wenhao Cui Yuanshuai Liu Pengfei Guo Zhijie Wu Liqun Kang Huawei Geng Shengqi Chu Linying Wang Dong Fan Zhenghao Jia Haifeng Qi Wenhao Luo Peng Tian Zhongmin Liu national engineering research center of Lower-Carbon Catalysis Technology Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of chinese Academy of Sciences Beijing 100049China Qingdao institute of Bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266101ShandongChina College of Chemistry and Chemical engineering Inner Mongolia UniversityHohhot 010021Inner MongoliaChina State Key Laboratory of heavy Oil Processing and Key Laboratory of Catalysis of CNPC China University of PetroleumBeijing 102249China Department of Inorganic Spectroscopy Max Planck Institute for Chemical Energy ConversionMülheim an der Ruhr 45470Germany Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China Division of energy research Resources Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Leibniz-Institut für Katalyse Albert-Einstein-Straβe 29aRostock 18059Germany

Zeolite-encapsulated metal nanoclusters are at the heart of bifunctional catalysts,which hold great potential for petrochemical conversion and the emerging sustainable ***,efficient encapsulation of metal nanoclusters into a high-silica zeolite Y in particular with good structural integrity still remains a significant ***,we have constructed Ru nanoclusters(~1 nm)encapsulated inside a high-silica zeolite Y(SY)with a SiO_(2)/Al_(2)O_(3) ratio(SAR)of 10 via a cooperative strategy for direct zeolite synthesis and a consecutive impregnation for metal *** with the benchmark Ru/H-USY and other analogues,the as-prepared Ru/H-SY markedly boosts the yields of pentanoic biofuels and stability in the direct hydrodeoxygenation of biomass-derived levulinate even at a mild temperature of 180℃,which are attributed to the notable stabilization of transition states by the enhanced acid accessibility and properly sized constraints of zeolite cavities owing to the good structural integrity.

关键词： High-silica zeolite Y metal encapsulation Bifunctional catalysis Hydrodeoxygenation Biofuels

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Direct generation of Zn metal using laser-induced ZnS to eradicate carbon emissions from electrolysis Zn production

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Frontiers of Environmental Science & engineering 2024年第1期18卷 83-95页

作者： Ying Chen Ning Duan Linhua Jiang Fuyuan Xu Guangbin Zhu Yao Wang Yong Liu Wen Cheng Yanli Xu State Key Laboratory of pollution control and Resources Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Shanghai institute of pollution control and Ecological Security Shanghai 200092China School of Environmental Science and engineering Tianjin UniversityTianjin 300350China School of Materials Science and engineering Anhui University of Science&TechnologyHuainan 232001China

In response to the goal of net-zero emissions proposed by Intergovernmental Panel on Climate Change, chinese government has pledged that carbon emissions will peak by 2030, and achieve carbon neutrality by 2060. However, the high carbon energy structure of traditional industries has aggravated environmental problems, such as greenhouse effect and air pollution. The goal of carbon neutrality will be difficult to achieve without the development of disruptive theories and technologies. The electrolytic zinc industry requires high-temperature roasting at ~1000 ℃, generating large amounts of greenhouse gases and SO_(2). High concentrations of sulfuric acid (200 g/L) are subsequently used for electrolysis, and each ton of zinc produced generates 50 kg of anode slime with lead content of up to 16%, as well as 0.35 m3 of wastewater containing zinc and lead. To solve these problems, an optical metallurgy method is proposed in this study. The proposed method uses laser-induced photoreduction to decompose ZnS and reduce metal ions to metal. Results indicate that Zn0 and S8 can be detected on the surface of ZnS at a specific wavelength and laser fluence. The generation mechanism of Zn0 is such that laser induces an electronic transition that breaks ionic bond in ZnS, resulting in its decomposition and photoreduction to Zn0 under an inert argon gas atmosphere. This method does not reduce other metals in the mineral since it does not use high-temperature roasting, providing a new way of producing high-purity metal without greenhouse gas emissions and heavy metal pollution caused by traditional zinc electrolysis.

关键词： Laser metallurgy ZnS Photochemical reduction Zinc

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