Metal organic framework derived Cu–carbon composite: An efficient non-noble metal catalyst for reduction of hexavalent chromium and pendimethalin

Zubair Hasan,최진우,Jörg Rinklebe,오용식,조동완,송호철 한국공업화학회 2017 Journal of Industrial and Engineering Chemistry Vol.52 No.-

A Cu–carbon composite was facilely synthesized via one step calcination of a Cu-based metal organicframeworks (MOF), HKUST-1, under N2 atmosphere. Physicochemical characteristics of the compositewere examined with a series of spectroscopy and surface analyzer. The composite was used as a catalystin the reduction of Cr(VI) and pendimethalin using HCOOH and NaBH4 as reductants, respectively. Thecomposite was very efficient in both reduction reactions, completing the reactions in several minutes. The composite also exhibited a robust reusability in the completion of four repeated Cr(VI) reductioncycles, demonstrating its potential utility as an alternative to noble-metal catalysts.

Recent advances in control technologies for non-point source pollution with nitrogen and phosphorous from agricultural runof: current practices and future prospects

Yinfeng Xia,Ming Zhang,Daniel C. W. Tsang,Nan Geng,Debao Lu,Lifang Zhu,Avanthi Deshani Igalavithana,Pavani Dulanja Dissanayake,Jörg Rinklebe,Xiao Yang,옥용식 한국응용생명화학회 2020 Applied Biological Chemistry (Appl Biol Chem) Vol.63 No.1

Eutrophication of natural water is a universal problem. Nitrogen (N) and phosphorus (P) from agricultural runoff are the main sources of nutrient input, provided that emissions from industrial point sources (IPS) are under control. Therefore, it is of great environmental importance to reduce pollution associated with agricultural runoff as a means of regulating eutrophication levels in natural water. Numerous methods proposed for treating agricultural runoff can be classified into three categories: source control, process control, and end treatment. In this review, major technologies for N and P control from agricultural runoff are summarized along with discussion of newly proposed technologies such as biochar biomimetics and microbial catalyst. Because agricultural runoff (from farmlands to receiving waters) is a complicated pollution process, it is difficult to regulate the nutrients discharged via such process. This review will thus offer a comprehensive understanding on the overall process of agricultural runoff and eutrophication to help establish control strategies against highly complicated agricultural non-point sources.

Metal organic framework derived Cu–carbon composite: An efficient non-noble metal catalyst for reduction of hexavalent chromium and pendimethalin

Hasan, Zubair,Cho, Jinwoo,Rinklebe, Jö,rg,Ok, Yong Sik,Cho, Dong-Wan,Song, Hocheol Elsevier 2017 Journal of industrial and engineering chemistry Vol.52 No.-

<P><B>Abstract</B></P> <P>A Cu–carbon composite was facilely synthesized via one step calcination of a Cu-based metal organic frameworks (MOF), HKUST-1, under N<SUB>2</SUB> atmosphere. Physicochemical characteristics of the composite were examined with a series of spectroscopy and surface analyzer. The composite was used as a catalyst in the reduction of Cr(VI) and pendimethalin using HCOOH and NaBH<SUB>4</SUB> as reductants, respectively. The composite was very efficient in both reduction reactions, completing the reactions in several minutes. The composite also exhibited a robust reusability in the completion of four repeated Cr(VI) reduction cycles, demonstrating its potential utility as an alternative to noble-metal catalysts.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Calcination of Cu-based metal organic framework (HKUST-1) to Cu–carbon composite. </LI> <LI> The composite showed high catalytic activity to reduce Cr(VI) and pendimethalin. </LI> <LI> The composite exhibited a robust reusability during repeated reduction cycles. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

N doped cobalt-carbon composite for reduction of <i>p</i>-nitrophenol and pendimethaline

Hasan, Zubair,Ok, Yong Sik,Rinklebe, Jö,rg,Tsang, Yiu Fai,Cho, Dong-Wan,Song, Hocheol Elsevier 2017 Journal of alloys and compounds Vol.703 No.-

<P><B>Abstract</B></P> <P>A novel and magnetically separable N doped-cobalt carbon composite (Co-NC) was facilely synthesized via thermal treatment of Co<SUB>3</SUB>O<SUB>4</SUB>-melamine mixture in atmospheric condition. The physicochemical properties of the composite were characterized with X-ray diffractometer, Raman spectroscopy, SQUID magnetometer, scanning electron microscope, and X-ray photoelectron spectroscopy. The catalytic ability of the composite was evaluated in reduction of <I>p</I>-nitrophenol and pendimethalin using NaBH<SUB>4</SUB> as a reductant. The composite showed a good catalytic performance to completely reduce 20 mg L<SUP>−1</SUP> of <I>p</I>-nitrophenol within 7.5 min, and 44 mg L<SUP>−1</SUP> of pendimethaline within 20 min at a dose of 0.27 mg mL<SUP>−1</SUP> and 0.32 mg mL<SUP>-1</SUP>, respectively. The composite also displayed a robust reusability with a small loss of catalytic activity in completion of four repetitive <I>p</I>-nitrophenol reduction cycles, demonstrating its potential utility as an alternative to noble-metal catalysts.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Magnetically separable N doped-cobalt carbon composite prepared via calcinations of Co<SUB>3</SUB>O<SUB>4</SUB> and melamine. </LI> <LI> Excellent performance for the reduction of <I>p</I>-nitrophenol and pendimethalin. </LI> <LI> First non-noble metal catalyst applied to catalytic reduction of pendimethalin. </LI> </UL> </P>

Modification of hydrothermal liquefaction products from <i>Arthrospira platensis</i> by using carbon dioxide

Choi, Dongho,Lee, Jechan,Tsang, Yiu Fai,Kim, Ki-Hyun,Rinklebe, Jö,rg,Kwon, Eilhann E. Elsevier Science B.V. Amsterdam 2017 Algal research Vol.24 No.1

<P><B>Abstract</B></P> <P>This study mainly reports that utilizing CO<SUB>2</SUB> as a reaction medium in hydrothermal liquefaction of <I>Arthrospira platensis,</I> as a model feedstock of microalgal biomass, provides a means for modifying the chemical constituents in microalgal bio-oil produced via hydrothermal liquefaction. Prior to hydrothermal liquefaction, the total lipid content of <I>A. platensis</I> was measured as ~3.5wt% (dry basis). Thermal degradation of <I>A. platensis</I> and the major pyrolytic gases from the thermal degradation of <I>A. platensis</I> were characterized to gain an insight into the physico-chemical influences of CO<SUB>2</SUB> in hydrothermal liquefaction. Based on the experiment's findings, hydrothermal liquefaction of <I>A. platensis</I> was conducted to evaluate the influence of CO<SUB>2</SUB>. Hydrothermal liquefaction of <I>A. platensis</I> in CO<SUB>2</SUB> decreased the composition of N-containing species from 63 to 59% and that of O-containing species from 31 to 27% in the bio-oil, significantly suggesting that using CO<SUB>2</SUB> improves the quality of bio-oil as a transportation fuel.</P> <P><B>Highlights</B></P> <P> <UL> <LI> CO<SUB>2</SUB> modifies N & O contents in <I>A. platensis</I>-bio-oil via hydrothermal liquefaction </LI> <LI> Liquefaction in CO<SUB>2</SUB> produces more CO from <I>A. platensis</I> </LI> <LI> Less N & O contained hydrocarbons produced from liquefaction of <I>A. platensis</I> in CO<SUB>2</SUB> </LI> </UL> </P>

Evaluating the feasibility of pyrophyllite-based ceramic membranes for treating domestic wastewater in anaerobic ceramic membrane bioreactors

Jeong, Yeongmi,Cho, Kyungjin,Kwon, Eilhann E.,Tsang, Yiu Fai,Rinklebe, Jö,rg,Park, Chanhyuk Elsevier 2017 Chemical engineering journal Vol.328 No.-

<P><B>Abstract</B></P> <P>This study laid great emphasis on anaerobic ceramic membrane bioreactor (AnCMBR) treatment of domestic wastewater for facile and enhanced energy recovery. To this end, the performance of the natural-based ceramic (<I>i.e.</I>, pyrophyllite-based) membranes was mainly explored in this study by evaluating filtration and treatment performances. 92.9±5.5% chemical oxygen demand (COD) removal and stable methane production were successfully achieved in a bench-scale AnCMBR while maintaining a slightly long hydraulic retention time (HRT). Comparative filtration experiments with commercialized ceramic membranes suggested that the pyrophyllite-based membrane separation in AnCMBR treatment of wastewater at long HRT is feasible. However, short HRT operations resulted in substantial levels of sludge washout. Future improvements of AnCMBR technology in cost-effective ceramic membrane development, increased flux, and harsh environmental conditions would make AnCMBR competitive with anaerobic membrane bioreactor (AnMBR) technology.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Pyrophyllite-based ceramic membranes applied to anaerobic membrane bioreactors. </LI> <LI> This novel approach achieved higher organic removal and methane yield at long HRTs. </LI> <LI> Short HRT operations resulted in substantial levels of sludge washout. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

Cadmium phytoremediation potential of <i>Brassica</i> crop species: A review

Rizwan, Muhammad,Ali, Shafaqat,Zia ur Rehman, Muhammad,Rinklebe, Jö,rg,Tsang, Daniel C.W.,Bashir, Arooj,Maqbool, Arosha,Tack, F.M.G.,Ok, Yong Sik Elsevier 2018 Science of the Total Environment Vol.631 No.-

<P><B>Abstract</B></P> <P>Cadmium (Cd) is a highly toxic metal released into the environment through anthropogenic activities. Phytoremediation is a green technology used for the stabilization or remediation of Cd-contaminated soils. <I>Brassica</I> crop species can produce high biomass under a range of climatic and growing conditions, allowing for considerable uptake and accumulation of Cd, depending on species. These crop species can tolerate Cd stress via different mechanisms, including the stimulation of the antioxidant defense system, chelation, compartmentation of Cd into metabolically inactive parts, and accumulation of total amino-acids and osmoprotectants. A higher Cd-stress level, however, overcomes the defense system and may cause oxidative stress in <I>Brassica</I> species due to overproduction of reactive oxygen species and lipid peroxidation. Therefore, numerous approaches have been followed to decrease Cd toxicity in <I>Brassica</I> species, including selection of Cd-tolerant cultivars, the use of inorganic and organic amendments, exogenous application of soil organisms, and employment of plant-growth regulators. Furthermore, the coupling of genetic engineering with cropping may also help to alleviate Cd toxicity in <I>Brassica</I> species. However, several field studies demonstrated contrasting results. This review suggests that the combination of Cd-tolerant <I>Brassica</I> cultivars and the application of soil amendments, along with proper agricultural practices, may be the most efficient means of the soil Cd phytoattenuation. Breeding and selection of Cd-tolerant species, as well as species with higher biomass production, might be needed in the future when aiming to use <I>Brassica</I> species for phytoremediation.</P> <P><B>Highlights</B></P> <P> <UL> <LI> <I>Brassica</I> species can be considered a potential candidate for Cd phytoremediation. </LI> <LI> <I>Brassica</I> species can accumulate most of the soil Cd in its parts. </LI> <LI> Different amendments can be applied to enhance Cd tolerance in <I>Brassica</I> species. </LI> <LI> Integrated agricultural practices can be used to enhance Cd uptake in <I>Brassica</I> species. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

Biochar affects the dissolved and colloidal concentrations of Cd, Cu, Ni, and Zn and their phytoavailability and potential mobility in a mining soil under dynamic redox-conditions

El-Naggar, Ali,Shaheen, Sabry M.,Ok, Yong Sik,Rinklebe, Jö,rg Elsevier 2018 Science of the Total Environment Vol.624 No.-

<P><B>Abstract</B></P> <P>There is a lack of knowledge on the effects of biochar (BC) on the release dynamics of potentially toxic elements (PTEs) in different phases of soil under systematic change of redox potential (E<SUB>H</SUB>). We aimed to elucidate the impact of pre-definite E<SUB>H</SUB> on the release dynamics of dissolved and colloidal concentrations of Cd, Cu, Ni, and Zn as well as their phytoavailability and potential mobility in the solid-phase of a mining soil treated with rice hull biochar (S+BC) compared to non-treated soil (S). The influence of E<SUB>H</SUB>-dependent changes of soil pH, dissolved organic carbon (DOC), dissolved aromatic carbon (DAC), Fe, Mn, SO<SUB>4</SUB> <SUP>2−</SUP>, and Cl<SUP>−</SUP> on the elements release was also determined. The experiment was conducted stepwise from reducing (−30mV in S and −12mV in S+BC) to oxidizing (+218mV in S and +333mV in S+BC) conditions using an automated biogeochemical microcosm system.</P> <P>Biochar-treated soil exhibited a wider range of E<SUB>H</SUB> and a lower pH than the non-treated soil. Dissolved concentrations of Cd, Cu, Ni, Zn, Fe, Mn, SO<SUB>4</SUB> <SUP>2−</SUP>, and DAC increased under oxic conditions in the non-treated and biochar-treated-soils, which might be due to the decline of pH, and/or sulfide oxidation. Cadmium was more abundant in the colloidal fraction, while Cu, Mn, and DOC were more abundant in the dissolved fraction. Nickel, Zn, and Fe distributed almost equally in both fractions. Biochar increased the dissolved concentration of Cd, Ni, Zn and in particular Cu under oxic conditions. However, the biochar did not significantly affect the colloidal fraction of Cd, Cu, Ni, and Zn. The phytoavailability of the studied elements was higher than the potential mobility. We conclude that increasing the dissolved concentrations of the elements under oxic conditions might increase their release and transfer into the groundwater and the food chain which should be harmful for the environment.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Biochar (BC) treated soil showed a wider range of E<SUB>H</SUB> and pH than the untreated soil. </LI> <LI> Biochar increased dissolved Cd, Cu, Ni, and Zn, particularly under oxic conditions. </LI> <LI> Cadmium was abundant in the colloidal and Cu in the dissolved fraction. </LI> <LI> Biochar increased dissolved Cd, Ni, Zn and in particular Cu under oxic conditions. </LI> <LI> The phytoavailability of the elements was higher than their potential mobility. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

Influence of bioenergy waste biochar on proton- and ligand-promoted release of Pb and Cu in a shooting range soil

Kumarathilaka, Prasanna,Ahmad, Mahtab,Herath, Indika,Mahatantila, Kushani,Athapattu, B.C.L.,Rinklebe, Jö,rg,Ok, Yong Sik,Usman, Adel,Al-Wabel, Mohammad I.,Abduljabbar, Adel,Vithanage, Meththika Elsevier 2018 The Science of the total environment Vol.625 No.-

<P><B>Abstract</B></P> <P>Presence of organic and inorganic acids influences the release rates of trace metals (TMs) bound in contaminated soil systems. This study aimed to investigate the influence of bioenergy waste biochar, derived from <I>Gliricidia sepium</I> (GBC), on the proton and ligand-induced bioavailability of Pb and Cu in a shooting range soil (17,066mg Pb and 1134mg Cu per kg soil) in the presence of inorganic (sulfuric, nitric, and hydrochloric) and organic acids (acetic, citric, and oxalic). Release rates of Pb and Cu in the shooting range soil were determined under different acid concentrations (0.05, 0.1, 0.5, 1, 5, and 10mM) and in the presence/absence of GBC (10% by weight of soil). The dissolution rates of Pb and Cu increased with increasing acid concentrations. Lead was preferentially released (2.79×10<SUP>−13</SUP> to 8.86×10<SUP>−13</SUP> molm<SUP>−2</SUP> s<SUP>−1</SUP>) than Cu (1.07×10<SUP>−13</SUP> to 1.02×10<SUP>−13</SUP> molm<SUP>−2</SUP> s<SUP>−1</SUP>) which could be due to the excessive Pb concentrations in soil. However, the addition of GBC to soil reduced Pb and Cu dissolution rates to a greater extent of 10.0 to 99.5% and 15.6 to 99.5%, respectively, under various acid concentrations. The increased pH in the medium and different adsorption mechanisms, including electrostatic attractions, surface diffusion, ion exchange, precipitation, and complexation could immobilize Pb and Cu released by the proton and ligands in GBC amended soil. Overall, GBC could be utilized as an effective soil amendment to immobilize Pb and Cu in shooting range soil even under the influence of soil acidity.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Presence of protons and ligands in soil increased the bioavailability of Pb and Cu. </LI> <LI> Biochar reduced Pb and Cu release rates to 99.5%. </LI> <LI> Electrostatic attraction and complexation to biochar could immobilize Pb and Cu. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>

Mechanistic insights into red mud, blast furnace slag, or metakaolin-assisted stabilization/solidification of arsenic-contaminated sediment

Wang, Lei,Chen, Liang,Tsang, Daniel C.W.,Zhou, Yaoyu,Rinklebe, Jö,rg,Song, Hocheol,Kwon, Eilhann E.,Baek, Kitae,Sik Ok, Yong Elsevier 2019 Environment international Vol.133 No.2

<P><B>Abstract</B></P> <P>Elevated level of arsenic (As) in marine sediment via deposition and accumulation presents long-term ecological risks. This study proposed a sustainable stabilization/solidification (S/S) of As-contaminated sediment via novel valorization of red mud waste, blast furnace slag and calcined clay mineral, which were selected to mitigate the increased leaching of As under alkaline environment of S/S treatment. Quantitative X-ray diffraction and thermogravimetric analyses illustrated that stable Ca-As complexes (e.g., Ca<SUB>5</SUB>(AsO<SUB>4</SUB>)<SUB>3</SUB>OH) could be formed at the expense of Ca(OH)<SUB>2</SUB> consumption, which inevitably hindered the hydration process and S/S efficiency. The <SUP>29</SUP>Si nuclear magnetic resonance analysis revealed that incorporation of metakaolin for As immobilization resulted in a low degree of hydration and polymerization, whereas addition of red mud promoted Fe-As complexation and demonstrated excellent compatibility with As. Transmission electron microscopy and elemental mapping further confirmed the precipitation of crystalline Ca-As and amorphous Fe-As compounds. Therefore, red mud-incorporated S/S binder achieved the highest efficiency of As immobilization (99.9%), which proved to be applicable for both <I>in-situ</I> and <I>ex-situ</I> S/S of As-contaminated sediment. These results advance our mechanistic understanding for the design of green and sustainable remediation approach for effective As immobilization.</P> <P><B>Highlights</B></P> <P> <UL> <LI> Stable Ca-As complexes could be formed at the expense of Ca(OH)<SUB>2</SUB> consumption. </LI> <LI> Metakaolin addition for S/S of As resulted in a low degree of hydration and polymerization. </LI> <LI> Incorporation of red mud promoted Fe-As complexation and improved compatibility with As. </LI> <LI> Green binders were applicable for both <I>in-situ</I> and <I>ex-situ</I> S/S of contaminated sediment. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>