SN Applied Sciences

, 2:184 | Cite as

Highly efficient removal of As(V) using metal–organic framework BUC-17

  • Da Pang
  • Peng Wang
  • Huifen Fu
  • Chen Zhao
  • Chong-Chen WangEmail author
Research Article
Part of the following topical collections:
  1. Materials Science: 2D Materials: Synthesis, Fundamental Properties, and Applications


Arsenic contamination is a great threat worldwide due to its toxicity and hardly degradable. The development of highly efficient adsorbents is an essential challenge in the water treatment field. A 2D metal–organic framework [Co3(tib)2(H2O)12](SO4)3 (BUC-17) has been synthesized by hydrothermal method, and was utilized as an efficient adsorbent to remove As(V) from contaminated water. The results showed that BUC-17 have higher adsorption capacity toward As(V) than most counterpart adsorbents, its maximum uptake capacity reached 129.2 mg g−1 at 298 K. The adsorption kinetics and isotherm behaviors were well fitted with pseudo-second-order and Langmuir model, respectively. The thermodynamic parameters such as free energy change ΔG°, enthalpy change ΔH° and entropy change ΔS° were both negative during the sorption process, suggesting that the adsorption process of BUC-17 towards As(V) was spontaneous and exothermal. The influence of pH and foreign ions on the adsorptive removal of As(V) using BUC-17 were investigated. The results showed that pH values have significant influence while co-existed anions (unless phosphate) exert slight effect on adsorption capacity. Finally, a corresponding adsorption mechanism was proposed and confirmed by scanning electron microscopy, Fourier Transform infrared spectra (FTIR) and X-ray photoelectron spectroscopy analysis.


BUC-17 Arsenic Adsorption Mechanism Performance 

1 Introduction

Arsenic is extensively distributed in the biosphere and has been linked with toxic and carcinogenic effects [1]. The chronical exposure to arsenic leads to nausea, cancer, muscular weakness, neurological disorder, appetite weakness and impairments of the immune system [2, 3, 4, 5]. Most arsenic compounds in the environment are discharged from coal combustion, production of industrial raw materials, arsenic pesticides, or volcano eruption [6, 7]. As a result of their strong toxicity and widely distribution, over 140 million people all over the world, especially in India, Bangladesh, Argentina, Vietnam and China, are facing the tremendous threat of arsenic [8, 9, 10]. The World Health Organization has regarded arsenic as a human carcinogen in drinking water and set a provisional standard of no more than 10 µg L−1 [11]. In natural waterbody, the arsenic exists in both inorganic arsenic compounds like arsenate, arsenite, and organic arsenic compounds like ASA (Arsanilic, C6H8AsNO3) and ROX (Roxarsone, C6H6AsNO6), in which As(V) is the primary arsenic species [12]. The existence of inorganic arsenic in natural water depends on the redox conditions. For example, As(V) will be converted into As(III) in the presence of reductive substances [13]. As well, it was well-recognized that the pre-oxidation of As(III) into As(V) is a necessary step for the efficiency of arsenic removal [14, 15]. Inorganic arsenic can be methylated in human body, which leads to the transformation from As(V) to As(III), resulting in a great potential threat to human health and environment [1, 16, 17]. Therefore, it is important to remove As(V) from polluted water.

Up to now, there are various techniques for arsenic removal like chemical precipitation, ion exchange, membrane filtration, biological processes and adsorption [3, 18, 19, 20], in which the adsorption is widely used in wastewater decontamination due to the advantages such as low cost, high speed, high efficiency and easy operation [21, 22, 23]. Traditional adsorbents including activated carbon [24], hydrotalcite [25], red mud [26] and activated alumina [27] are facing problems like low adsorption capacity. It was urgent and essential to develop new adsorbent materials with high efficiency to eliminate arsenic in wastewater.

Metal–organic frameworks (MOFs) are unique porous crystalline materials with large surface area, abundant binding site, regular channel, and tunable morphology, which are widely used in the fields of photocatalysis, adsorption, gas storage and separation [28, 29, 30, 31, 32]. Adsorptive removal of arsenic using MOFs have attracted extensive attentions due to their outstanding adsorption capacity, high removal efficiency, short reaction time and wide range of suitable pH values [7, 12, 33, 34]. Furthermore, MOFs possess abundant metal sites even unsaturated coordination sites, which can be coordinated with arsenic for enhanced adsorption ability [35, 36]. However, many MOFs are not stable in water, which exerted great difficulty to carry out reuse and recyclability [37].

A new 2D metal–organic framework [Co3(tib)2(H2O)12](SO4)3 (BUC-17) has been synthesized from tib (1,3,5-tris(1-imidazolyl)benzene) and Co2+ by hydrothermal methods, which exhibited ultrahigh adsorption capacity towards some organic dyes [38] as well as Cr(VI) [39]. Considering that BUC-17 displayed preferential uptake to anionic matters, it was used to carry out adsorptive removal toward As(V) in HAsNa2O4. Also, the corresponding kinetics, isotherms and the thermodynamic parameters were fitted and calculated. Finally, the adsorption mechanism between BUC-17 and As(V) was proposed, and confirmed by scanning electron microscopy (SEM), Fourier Transform infrared spectra (FTIR) and X-ray photoelectron spectra (XPS) analyses.

2 Materials and methods

2.1 Synthesis of BUC-17

All the chemicals were reagent grade and used without further purification. BUC-17 was synthesized following the reported method [38, 39] with minor modification. Briefly, CoSO4·7H2O (0.3 mmol, 0.0843 g) and 1,3,5-tris(1-imidazolyl)benzene (tib) (0.3 mmol, 0.0828 g) were mixed with 10 mL deionized water and then added 5 mL ethanol (99%) in a 25 mL Teflon-lined stainless steel Parr bomb, and heated in a drying oven at 413 K for 72 h. The pink powders are acquired by filtration, and then washed three times using deionized water and ethanol (99%) in turn to obtain pure BUC-17.

2.2 Characterization

The Fourier transform infrared (FTIR) spectra were used to analyze the change of adsorbent throughout the whole adsorption process by a Nicolet 6700 FTIR spectrometer with KBr pellets in the range of 4000–400 cm−1. The morphologies and the elemental mappings for adsorbent BUC-17 before and after adsorption were acquired on a FEI Quanta 250 FEG scanning electron microscope (SEM) equipped with Bruker XFlash 5010 Energy Dispersive Spectrometer (EDS). The change of crystalline structures and compositions of the before and after adsorbed samples were characterized by powder X-ray diffraction (PXRD) under Cu Kα radiation in the 2θ range of 5°–50° on Dandonghaoyuan DX-2700B diffractometer. X-ray photoelectron spectra (XPS) measurement was carried out on Thermo ESCALAB 250XI to determine adsorbent with its chemical valence state and composition.

2.3 Adsorption experiments

An aqueous stock solution of As(V) (500 mg L−1) was prepared by dissolving HAsNa2O4·7H2O (SIGMA, 98%, 0.5206 g) in deionized water (250 mL), and then stored in the dark at 277 K. The pH values of As(V) solution were adjusted by using aqueous NaOH (0.1 M) or HCl (0.1 M) solution. 40 mg BUC-17 samples were added to 200 mL of As(V) solution with initial concentrations of 5 mg L−1 to 100 mg L−1. The mixtures were placed on the constant temperature shaker under speed of 170 r min−1 at 298 K, 303 K, 308 K. During the shaking process, 5 mL samples were drawn from the suspensions and then separated by a 0.22 µm membrane filter for further analysis. The residual As(V) concentration was analyzed by ICP-OES (ICP-5000, Focused Photonics (Hangzhou) Inc). The adsorption capacity q (mg g−1) was obtained by Eq. (1):
$$q = (C_{0} - C_{{\text{e}}} )V/m$$

where, C0 and Ce are the initial and equilibrium concentrations (mg L−1) of As(V), respectively; V is the solution volume (L) and m is the dosage of the adsorbent (g).

3 Results and discussion

3.1 Adsorption kinetics

In order to determine the effect of contact time on adsorption process of As(V) by BUC-17, it was necessary to conduct series of experiments to study the adsorption kinetics. 40 mg BUC-17 samples were added to 200 mL As(V) solution with initial concentrations ranging from 5 mg L−1 to 100 mg L−1 (pH = 10) at 298 K for 48 h. The relationships between adsorption capacity and constant time are given in Fig. 1. The maximum adsorption capacity of BUC-17 toward AS(V) was 129.2 mg g−1, which was higher than those of counterpart adsorbents like MIL-53(Al) [18], ZIF-8 [37] and other MOFs as listed in Table 1. For the initial As(V) concentrations of 50 and 100 mg L−1, 90% equilibrium adsorption capacities were achieved within first 3 h, and the adsorption equilibrium was accomplished for As(V) solution with concentration of 50 and 100 mg L−1within 12 h. To analyze adsorption kinetics and describe the adsorption behaviors, the pseudo first-order [27] and pseudo second-order kinetic [12, 40] models (Eqs. (2) and (3)) were fitted to the kinetic data.
$${\ln}\,(q_{{\text{e}}} - q_{{\text{t}}} ) = {\ln}\,(q_{{\text{e}}} ) - K_{{1}} t$$
$$t/q_{{\text{t}}} = 1/(K_{{2}} q_{{\text{e}}}^{{2}} ) + \, t/q_{{\text{e}}}$$
Fig. 1

The adsorption capacities of BUC-17 toward As(V) with different initial concentrations (pH = 10.0, T = 298 K)

Table 1

The adsorption capacities of different adsorbents toward As(V)


Adsorption capacity (mg g−1)

Equilibrium time




24 h


ZIF-8 nanoparticles


24 h


Hierarchical ZIF-8






48 h








20 min






MIL-88A microrods


12 h














MOF-808 nanoparticles






24 h




12 h

This work

where, qe and qt (mg g−1) are the adsorption quantities of As(V) at equilibrium time and at a sometime t, respectively. K1 (min−1) and K2 (g mg−1 min−1) are the adsorption rate constants of the pseudo first-order and the pseudo-second-order adsorption, respectively.

From Fig. 2 and Table 2, it can be observed that the adsorption process were better fitted in the pseudo-second-order kinetic models, owing to higher correlation coefficient and narrow difference between the experimental and theoretical values of equilibrium adsorption capacity. It indicated that the rate-limiting step might be chemisorption [7]. Furthermore, to investigate the effect of intraparticle diffusion and ensure the rate limiting step, the Weber–Morris model [46] as represented by Eq. (4) was used to process the kinetics data.
$$q_{{\text{t}}} = Kt^{{{1}/{2}}} + \, C$$
Fig. 2

a Pseudo-first-order kinetic and b pseudo-second-order kinetic models for adsorption process of BUC-17 towards As(V) at 298 K

Table 2

Kinetic parameters of pseudo-first-order and pseudo-second-order models for fitting kinetic data of As(V) adsorption with different concentration onto BUC-17 (298 K)

C0 (mg g−1)



Experimental value q (mg g−1)

K1 (min−1)

qe (mg g−1)


K2 (g mg−1 min −1)

qe (mg g−1)


























































where, K (mg g−1 min−1/2) is the intraparticle diffusion rate constant. The adsorption process could be mainly divided into two sub-processes as shown in Fig. 3. Firstly, the part of steeper slope with faster adsorption rate corresponds to external transfer step, in which the As(V) is adsorbed onto the external surface of BUC-17. Secondly, the adsorbed As(V) is further spread from the surface to the internal active sites of BUC-17 until the adsorption equilibrium is reached, which corresponds to the intraparticle diffusion and equilibrium step. The second step is generally slow evidenced by small adsorption rate [12]. It is worthy to note that the higher initial As(V) concentration results into the faster adsorption rate of external transfer step (first step), due to the fact that the higher initial concentrations can enhance diffusion driving force [12, 36].
Fig. 3

The Weber–Morris model for adsorption process of BUC-17 towards As(V) at 298 K

3.2 Adsorption isotherms

To explore the relationship between temperature and adsorption capacity, series experiments were performed by adding 40 mg BUC-17 samples to 200 mL As(V) solution with various initial concentrations (5–100 mg L−1) at pH = 10. The suspensions were stirred at speed of 170 r min−1 during the test in the shaker for 48 h to reach adsorption equilibrium at 298 K, 303 K and 308 K, respectively. The different isotherm models like Langmuir [47], Freundlich [48] and Dubinin–Radushkevich [49] (D-R) were adopted to explain the adsorption modes between adsorbent BUC-17 and adsorbates As(V). The Langmuir, Freundlich and Dubinin–Radushkevich (D–R) isotherm models are demonstrated in Eqs. (5), (6) and (7), respectively.
$$C_{{\text{e}}} /q_{{\text{e}}} = 1/K_{{\text{L}}} q_{{\max}} + C_{{\text{e}}} /q_{{\max}}$$
$${\log}q_{{\text{e}}} = {\log}K_{{\text{f}}} + ({1}/n){\log}C_{{\text{e}}}$$
$${\ln}\,q_{e} = {\ln}\,q_{{\max}} - K_{DR} \xi^{{2}}$$
where, qmax (mg g −1) is the theoretical maximum adsorption capacity toward As(V); KL is the Langmuir constant, which is related to adsorption energy; qe (mg g−1) is the adsorption amount reaching adsorption equilibrium; Ce (mg L−1) is the equilibrium As(V) concentration; Kf (mg g −1) is the Freundlich constants, which indicates the adsorption ability of adsorbent; n is a constant related to system degree for adsorption; KDR (mol2 J−2) is the D–R constant related to average sorption energy; ξ (J mol−1) and E (kJ mol−1) represents the Polanyi potential and adsorption free energy, respectively, which can be calculated by using Eqs. (8) and (9).
$$\xi = RT{\ln}\left( {{1} + {1}/C_{{\text{e}}} } \right)$$
$$E = {1}/\left( {{2}K_{{{\text{DR}}}} } \right)^{{{1}/{2}}}$$
To clarify the adsorption mechanism of BUC-17 toward As(V), the adsorption isotherms data were fitted with three isotherm models as shown in Fig. 4. The adsorption isotherm parameters are given in Table 3. It is clearly that the adsorption process was suitably fitted in Langmuir adsorption isotherm models with R2 values over 0.99, which are well consistent with the adsorption process of BUC-17 towards organic dyes [38] and Cr(VI) [39] as well as other adsorbents towards arsenic [7, 36], suggesting that the adsorption process is monolayer adsorption [43]. With the increase of temperature, the maximum adsorption capacity and Langmuir constant decreases continuously. Therefore, the adsorption process is an exothermic process, which was favorable at low temperature.
Fig. 4

The a Equilibrium data for As(V) adsorption by BUC-17 at different temperatures. b Langmuir, c Freundlich, and d Dubinin–Radushevich (D–R) adsorption isotherm models for adsorption of As(V) onto BUC-17

Table 3

Constants of Langmuir, Freundich, and D–R for As(V) adsorption by BUC-17 at different temperatures





KL(L mg−1)

qm (mg g−1)


Kf (L g−1)




E (KJ mol−1)









3.98 \(\times\) 10–4










4.13 \(\times\) 10–4










8.04 \(\times\) 10–4



3.3 Thermodynamic calculations

The thermodynamic parameters which include standard Gibbs free energy (ΔG°, kJ mol−1), entropy change (ΔS°, J mol−1 K−1) and enthalpy change (ΔH°, kJ mol−1) were calculated to get further insight into feasibility, favorability, and spontaneity of the adsorption process. They can be respectively calculated with the aid of data obtained from Langmuir adsorption isotherm via Eqs. (10) and (11) [50].
$$\Delta G^\circ = - RT{\ln}\,K$$
$${\ln}\,K = \Delta S^\circ /R - \Delta H^\circ /RT$$
where, T (K) is the Kelvin temperature, R (8.314 kJ mol−1 K−1) is the universal gas constant and K is equilibrium coefficient estimated by the Langmuir parameter (KL) [51] as Eq. (12):
$$K = K_{{\text{L}}} C_{{\text{w}}}$$

where, Cw (1.01 \(\times\) 106 mg L−1) represents the water concentration.

All the calculated thermodynamic parameters are illustrated in Table 4. In general, the free energy (ΔG°) values ranging from – 20 to 0 kJ mol−1 indicate that physi-sorption process predominates. While, ΔG° values between − 80 to − 400 kJ mol−1 suggest chemisorption process [52]. In this study, the ΔG° values are − 30.84 kJ mol−1, − 30.76 kJ mol−1, − 30.50 kJ mol−1 at 298 K, 303 K, 308 K, respectively, suggesting that physi-sorption process dominates in parallel with partial chemical sorption [52, 53]. Furthermore, the negative ΔG° values indicated that the adsorption process was a spontaneous process. The higher temperature led to declining adsorption capacity, which was confirmed by the maximum adsorption capacities of BUC-17 decreasing from 134.96 mg g−1 at 298 K to 131.23 mg g−1 at 308 K. The value of ΔH° (−40.80 kJ mol−1) suggests that the adsorption reaction is exothermic, while the negative of ΔS° value (− 33.22 J mol−1 K−1) implies that the randomness decreased after the adsorption process. All the thermodynamic parameters reveal that the adsorption processes are spontaneous and exothermic.
Table 4

Thermodynamic parameters for As(V) adsorption via BUC-17 at different temperatures



ΔG° (kJ mol −1)

ΔS° (J mol−1 K−1)

ΔH° (kJ mol−1)



− 30.84

− 33.32

− 40.80



− 30.76



− 30.50

3.4 Influencing factors

3.4.1 Effect of pH

The pH value of As(V) solution is an extreme important factor to influence the adsorption process, because it determines the anionic species of arsenic along with the surface changes and the ionization of adsorbents [54, 55]. The effect of pH on the adsorption capacity was investigated in the pH range of 4.0–10.0, in which 40.0 mg BUC-17 were added to 200 mL As(V) solution with initial concentration of 10 mg L−1 under 298 K. As shown in Fig. 5a, the As(V) removal efficiency decrease dramatically from 10% at pH = 4.0 or 5.0 to 80% at pH = 10.0, which can be contributed to both the decreasing zeta potential of BUC-17 and the different anionic species of As(V) in solution. The mainly anionic species of As(V) in solution under different pH values are H3AsO4 (pH < 2.3), H2AsO4 (3 < pH < 6), HAsO42− (8 < pH < 10.5), AsO43− (pH > 11) [56, 57]. With the increase of pH from 4.0 to 10.0, the average number of negative charge of arsenate increases, which has positive effect on electrostatic attraction [57, 58]. Meanwhile, the zeta potential of BUC-17 decreases from 4.0 to 10.0 [39], which leads to the gradually decreased area occupied by the average single arsenate adsorption, and exerts negative effect on electrostatic attraction. Finally, the combination of the two interactions leads to an enhancement of the adsorption capacity in total [43].
Fig. 5

a The adsorption capacity of BUC-17 toward As(V) under various pH values; b The adsorption capacity of BUC-17 toward As(V) in the presence of different coexisting anions

3.4.2 Effect of coexisting anions

It is generally known that the co-existing anions in solution like nitrate, chlorate and phosphate are important factors in estimating its practical applicability as adsorbent [7]. To explore the effect of coexisting anions in As(V) solution, the experiment was demonstrated by adding 40 mg BUC-17 into 200 mL solution containing 10 mg L−1 of As(V) solution (pH = 10) with and without coexistent anions like NO3, F, Cl, SO42−, PO43− at 298 K. The concentration of all coexisting anions was 0.02 mol L−1. The adsorption capacity ratio (%) are removal ratio without coexistent anions divide by removal ratio with coexistent anions. As shown in Fig. 5b, only 13.4% of the adsorption capacity was maintained in the presence of PO43−, which may be due to phosphate and arsenate have similar adsorption behavior [59] and phosphate is more competitive for binding sites of BUC-17 [37]. On the contrary, other co-existed anions like NO3, F, Cl, SO42− exert no significant effect on adsorption capacity, which indicates that BUC-17 displayed good adsorption efficiency in the presence of different anions unless phosphate.

3.5 Proposed adsorption mechanism

In order to confirm adsorption mechanism, the elemental mappings, FTIR spectra and XPS of BUC-17 were obtained before and after As(V) adsorption. As shown in Fig. 6, the elemental mapping obtained from SEM verified the presence of As in BUC-17 after adsorbing As(V) besides Co, O, N, S and C. What’s more, the uptake of As(V) onto BUC-17 can be also affirmed by FTIR spectra in Fig. 7b as a new adsorption band appeared at 881 cm−1 which corresponds to the stretching vibration of As-O bond for BUC-17 after adsorption [7, 60]. Furthermore, the main peaks of BUC-17 before and after adsorption matched well in PXRD patterns as shown in Fig. 7a, the peaks of As(V)-loaded BUC-17 were lower than the pristine BUC-17, as a result of the surface of BUC-17 covered with the adsorbed As(V), which affirmed a good stability of BUC-17 during the adsorption process [36].
Fig. 6

Elemental mapping of BUC-17 before and after adsorption toward As(V)

Fig. 7

a The PXRD patterns of BUC-17 before and after adsorption toward As(V); b The FTIR spectra of BUC-17 before and after adsorption toward As(V)

The BET surface area of BUC-17 is 2.39 m2 g−1 and the pore size of BUC-17 is ca. 2.36 nm [38], indicating that its highly efficient adsorption towards arsenate might not be attributed to its porosity. As previously reported by Li et al. and Guo et al., BUC-17 has an overall positive surface charge from pH = 4 to pH = 10 [38, 39], demonstrating that electrostatic interaction contributed to the adsorption process of As(V) by BUC-17. In addition, the decrease of S element accompanied with the increase As element after adsorption were obtained from SEM indicated that ion-exchange interactions exist in the adsorption process. The experiment was conducted to study adsorption capacity towards As(V) in saturated aqueous Na2SO4 solution and in pure aqueous solution. As illustrated in Fig. 8f, the presence of SO42− obviously inhibited the As(V) adsorption onto BUC-17, as confirmed by the removal efficiency decrease from 94.6% (without Na2SO4 aqueous solution) to 79.8% (saturated Na2SO4 aqueous solution) with initial solution concentration of 5 mg L−1. What’s more, the decrease of the uncoordinated SO42− from BUC-17 was evidenced by XPS, in which the binding energy of 168.22 eV (S 2p) belonging to SO42− decreased sharply. Meanwhile, a new As 2p (1326.74 eV) peaks of arsenate emerged after adsorption, suggesting that ion-exchange interactions played an important role in the adsorption process [61, 62]. Therefore, the possible adsorption mechanism of As(V) onto BUC-17 were ion-exchange interactions and electrostatic interaction as illustrated in Fig. 9.
Fig. 8

a Full range XPS spectra of BUC-17 before and after As(V) adsorption; b XPS spectra of As 2p before and after As(V) adsorption; c XPS spectra of S 2p before and after As(V) adsorption; d XPS spectra of Co 2p before and after As(V) adsorption; e XPS spectra of O 1 s before and after As(V) adsorption; f Adsorption of As(V) in deionized water and in saturated Na2SO4 solution with BUC-17

Fig. 9

Proposed interaction mechanism between As(V) and BUC-17

4 Conclusion

In this study, BUC-17 exhibited good adsorption performance for the As(V) removal from wastewater; the adsorption kinetics and adsorption isotherm of As(V) on BUC-17 were suitably fitted by the pseudo-second-order kinetic model, and Langmuir isotherm model, respectively, and the maximum adsorption capacity was 129.2 mg g−1, higher than most reported adsorbents for As(V) removal. The adsorption process was spontaneous, exothermic and the randomness decreased as the result of negative ΔG°, ΔH° and ΔS° values. The pH values and foreign ions were also important influence factors during the whole adsorption process. The possible adsorption mechanisms in this study were proposed, including electrostatic and ion-exchange interactions. With the good adsorption performance towards As(V), BUC-17 could be potentially applied in industrial wastewater treatment.



The authors acknowledge financial support from Project of the National Science Foundation of China (51878023,51578034), Construction of Innovation Teams and Teacher Career Development for Universities and Colleges Under Beijing Municipality (IDHT20170508), Great Wall Scholars Training Program Project of Beijing Municipality Universities (CIT&TCD20180323), Beijing Talent Project (2019A22), the Fundamental Research Funds for Beijing Universities of Civil Engineering and Architecture (X18276) and Scientific Research Foundation of Beijing University of Civil Engineering and Architecture (KYJJ2017008).

Compliance with ethical standards

Conflict of interest

The authors declare that they have no conflict of interest.


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Copyright information

© Springer Nature Switzerland AG 2020

Authors and Affiliations

  • Da Pang
    • 1
  • Peng Wang
    • 1
  • Huifen Fu
    • 1
  • Chen Zhao
    • 1
  • Chong-Chen Wang
    • 1
    Email author
  1. 1.Beijing Key Laboratory of Functional Materials for Building Structure and Environment Remediation/Beijing Advanced Innovation Centre for Future Urban DesignBeijing University of Civil Engineering and ArchitectureBeijingChina

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