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Tiêu đề Recombinant Derivatives Of The Human High-Mobility Group Protein HMGB2 Mediate Efficient Nonviral Gene Delivery
Tác giả Arjen Sloots, Winfried S. Wels
Trường học Chemotherapeutisches Forschungsinstitut, Georg-Speyer-Haus
Chuyên ngành Gene Therapy
Thể loại báo cáo khoa học
Năm xuất bản 2005
Thành phố Frankfurt am Main
Định dạng
Số trang 16
Dung lượng 559,97 KB

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Nội dung

HMGB2186facilitates gene delivery into COS-7 cells To investigate HMGB2186-mediated gene transfer, the pCMS-eGFP-E2C-Luc reporter gene plasmid was used which encodes enhanced green fluore

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protein HMGB2 mediate efficient nonviral gene delivery Arjen Sloots and Winfried S Wels

Chemotherapeutisches Forschungsinstitut, Georg-Speyer-Haus, Frankfurt am Main, Germany

Virus-based vectors have been the gene delivery

vehi-cles of choice in most gene therapy approaches to date,

and use of these vectors has led to significant successes

in a number of clinical trials [1] Nevertheless, recent

adverse events in patients treated with different viral

vectors have revived interest in alternative, nonviral

delivery systems for gene therapy [2,3] Although still

less efficient than most viral vectors, nonviral gene

delivery vehicles are not usually associated with serious

safety concerns

In addition to synthetic nonviral vectors such as

lipids and polycationic reagents, certain natural

peptides and proteins are able to bind and condense plasmid DNA, a prerequisite for the formation of transfection-competent complexes [4] Consequently, cellular DNA-binding proteins including histones [5–9] and high-mobility group (HMG) proteins [10,11] have been investigated for their potential as nonviral gene delivery reagents In these studies, DNA-binding pro-teins were extracted from tissues such as calf thymus, which requires large amounts of starting material and can yield heterogeneous protein fractions that display reduced DNA-binding activity because of exposure to acid during purification [12,13] Therefore recombinant

Keywords

gene delivery; high-mobility group protein;

importin-a; nuclear localization signal;

protein transduction domain

Correspondence

W S Wels, Chemotherapeutisches

Forschungsinstitut, Georg-Speyer-Haus,

Paul-Ehrlich-Straße 42–44, D-60596

Frankfurt am Main, Germany

Fax: +49 69 63395 189

Tel: +49 69 63395 188

Email: wels@em.uni-frankfurt.de

(Received 13 April 2005, revised 23 June

2005, accepted 24 June 2005)

doi:10.1111/j.1742-4658.2005.04834.x

Certain natural peptides and proteins of mammalian origin are able to bind and condense plasmid DNA, a prerequisite for the formation of transfec-tion-competent complexes that facilitate nonviral gene delivery Here we have generated recombinant derivatives of the human high-mobility group (HMG) protein HMGB2 and investigated their potential as novel protein-based transfection reagents A truncated form of HMGB2 encompassing amino acids 1–186 of the molecule was expressed in Escherichia coli at high yield This HMGB2186 protein purified from bacterial lysates was able to condense plasmid DNA in a concentration-dependent manner, and medi-ated gene delivery into different established tumor cell lines more efficiently than poly(l-lysine) By attaching, via gene fusion, additional functional domains such as the HIV-1 TAT protein transduction domain (TATPTD -HMGB2186), the nuclear localization sequence of the simian virus 40 (SV40) large T-antigen (SV40NLS-HMGB2186), or the importin-b-binding domain (IBB) of human importin-a (IBB-HMGB2186), chimeric fusion pro-teins were produced which displayed markedly improved transfection effi-ciency Addition of chloroquine strongly enhanced gene transfer by all four HMGB2186derivatives studied, indicating cellular uptake of protein–DNA complexes via endocytosis The IBB-HMGB2186 molecule in the presence

of the endosomolytic reagent was the most effective Our results show that recombinant derivatives of human HMGB2 facilitate efficient nonviral gene delivery and may become useful reagents for applications in gene therapy

Abbreviations

eGFP, enhanced green fluorescent protein; HMG protein, human high-mobility group protein; IBB, importin-b-binding domain; NLS, nuclear localization sequence; PEI, polyethyleneimine; PTD, protein transduction domain; SV40, simian virus 40.

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DNA-binding proteins such as human histone H1

expressed in bacteria and rat HMGB1 produced in

yeast cells are suitable alternatives [12,14]

On its own the ability of a nonviral vector to

con-dense DNA is not sufficient to mediate gene delivery

with high efficiency Eukaryotic cells are protected

against the uptake of exogenous nucleic acids by a

series of cellular barriers that must be overcome before

a delivered gene can be expressed in the target cell

nucleus In particular, ineffective escape from

endo-somal compartments and poor nuclear trafficking are

considered major limiting factors for many nonviral

gene-transfer systems [15,16] The production of

pro-tein-based gene-delivery vectors in recombinant form

in principle allows their activities to be modified by

inclu-ding heterologous sequences that help to overcome

these cellular barriers by improving cellular uptake,

endosome escape, and intracellular routing [17]

Here we report the construction of recombinant

derivatives of the human nonhistone chromatin protein

HMGB2 and their functional characterization as

non-viral gene delivery vectors Vertebrate HMGB proteins

such as HMGB1 and HMGB2 are composed of three

structurally defined regions [18,19] They contain two

homologous but distinct DNA-binding motifs, termed HMG boxes, and an acidic C-terminal domain In human HMGB2, the HMG boxes A and B, inter-spaced by basic amino acids, are connected by another basic region to a stretch of 22 acidic amino acids at the C-terminus of the protein [20,21] (schematically shown in Fig 1A) These basic regions together with some basic amino-acid residues at the N-terminus of HMG box A have been suggested to function as a nuclear localization signal (NLS) [22]

We generated a truncated HMGB2 derivative which lacks the acidic tail previously reported to decrease the affinity of HMG proteins for DNA [23] This bacterially expressed HMGB2186 fragment formed complexes with plasmid DNA, and mediated gene delivery into different established tumor cell lines more efficiently than poly(l-lysine) Further-more, by including additional functional domains such as the HIV-1 TAT protein transduction domain (PTD), the NLS of the simian virus 40 (SV40) large T-antigen, or the importin-b-binding domain (IBB)

of human importin-a2, alternative gene delivery vec-tors were produced that displayed markedly enhanced transfection efficiency

A

B

Fig 1 Construction and bacterial expression of HMGB2 186 (A) Schematic representation of the human HMGB2 protein and the expression construct encoding truncated HMGB2186 Full-length HMGB2 consists of HMG box A, a linker region (L), HMG box B, a joiner region (J) and

an acidic C-terminal tail The bacterial expression vector pSW5-HMGB2186encodes under the control of the isopropyl b- D -thiogalactopyrano-side-inducible tac promoter (tac) amino acids 1–186 of human HMGB2 fused to C-terminal Myc (M) and polyhistidine (H) tags (B) SDS ⁄ PAGE (lanes 1–4) and immunoblot analysis (lanes 5–8) of bacterial lysate (lanes 1, 5), flow through (lanes 2, 6), wash (lanes 3, 7) and eluate fraction (lanes 4, 8) during purification of HMGB2186by Ni 2+ affinity chromatography HMGB2186was identified with Myc-tag-specific antibody 9E10 followed by horseradish peroxidase-coupled secondary antibody and chemiluminescent detection.

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Truncated human HMGB2186is readily expressed

in bacteria

For bacterial expression of a truncated derivative of

HMGB2 that lacks the acidic tail, a cDNA fragment

encoding amino acids 1–186 (HMGB2186) was derived

by PCR and inserted into the expression vector pSW5

[24] In the resulting pSW5-HMGB2186 plasmid,

cyto-plasmic expression of HMGB2186 fused to C-terminal

Myc and His-tags is controlled by an isopropyl

b-d-thio-galactopyranoside-inducible tac promoter (Fig 1A)

HMGB2186 protein was expressed in Escherichia coli

strain BL21(kDE3)trxB–[25] and purified from bacterial

lysates under native conditions by Ni2+-affinity

chro-matography as described in Experimental Procedures

In SDS⁄ PAGE analysis, purified HMGB2186 could be

detected as a single band with an apparent molecular

mass slightly larger than calculated from its sequence

(24.2 kDa; Fig 1B) Similar results were obtained in

immunoblot analysis with mAb 9E10 specific for the

Myc tag included in the molecule, further confirming

the identity of the recombinant protein (Fig 1B)

Recombinant HMGB2186binds to plasmid DNA

and cell surfaces

Binding of HMGB2186 protein to plasmid DNA was

investigated in a gel retardation experiment (Fig 2A)

Increasing amounts of purified HMGB2186 were

incu-bated with 0.5 lg reporter gene plasmid

pCMS-eGFP-E2C-Luc The electrophoretic mobility of the resulting

protein–DNA complexes in 1% agarose gel was then

determined In the absence of HMGB2186, plasmid

DNA migrated as expected, with supercoiled and

relaxed forms as separate bands (Fig 2A, lane 1) The

addition of 0.7 or 1.4 lg HMGB2186 already retarded

the plasmid DNA substantially (Fig 2A, lanes 3, 4),

and with 2.8 lg or more, maximal retardation of

plas-mid DNA was achieved (Fig 2A, lane 5) In contrast,

BSA, included as a control protein, had no effect on

the electrophoretic mobility of plasmid DNA Plasmid

DNA in HMGB2186 complexes containing 2.8 lg or

more purified protein similar to DNA in poly(l-lysine)

complexes was completely protected against

degrada-tion by DNase I (data not shown)

Another important determinant of successful gene

delivery is the binding of DNA–vector complexes to

target cells This can occur by direct interaction of

transfection complexes with integral components of

the cell membrane, or by binding to other molecules

expressed on the cell surface [15,16] Binding of recom-binant HMGB2186 to target cells was investigated by FACS analysis using human HeLa cells and COS-7 African green monkey kidney cells as a model The cells were incubated with increasing concentrations of purified HMGB2186, and bound protein was detected with mAb 9E10 recognizing the Myc tag included in the molecule, followed by fluorescein isothiocyanate-conjugated or phycoerythrin-isothiocyanate-conjugated secondary anti-bodies As shown in Fig 2B, concentration-dependent and saturable binding of HMGB2186to the cell surface was detected, suggesting specific interaction with an as yet unidentified target molecule

HMGB2186facilitates gene delivery into COS-7 cells

To investigate HMGB2186-mediated gene transfer, the pCMS-eGFP-E2C-Luc reporter gene plasmid was used which encodes enhanced green fluorescent protein (eGFP) and an optimized form of firefly luciferase under the control of the SV40 enhancer⁄ promoter and the cytomegalovirus immediate early promoter, respectively Transfection complexes containing increasing amounts

of purified HMGB2186protein and 2.3 lg pCMS-eGFP-E2C-Luc DNA were added to COS-7 cells in standard growth medium with serum, and left on the cells for 4 h before the medium was exchanged Cells were lysed 40 h later, and luciferase activity was measured For compar-ison, control cells were transfected with poly(l-lysine)– DNA complexes containing 2.3 lg reporter plasmid and a 60-fold molar excess of poly(l-lysine) as described [26] The results are shown in Fig 2C Concentration-dependent HMGB2186-mediated gene delivery was found, which was more efficient than poly(l-lysine)-mediated transfection at an HMGB2186 amount of 21.5 lg (representing a protein⁄ DNA mass ratio of 9.5)

or higher In this experiment, maximal reporter gene expression was reached with 43 lg HMGB2186, with luciferase activity eight times higher than in the poly (l-lysine) control Interestingly, in COS-7 cells, effi-ciency of HMGB2186-mediated gene transfer decreased again at higher HMGB2186 concentrations, possibly because of saturation of cell surface molecules occupied

by excess free HMGB2186protein

To investigate the possible involvement of the endo-cytic pathway in the internalization of HMGB2186– DNA complexes, cells were also transfected in the presence of the endosomolytic agent chloroquine [27,28] As shown in Fig 2D, the efficiency of HMGB2186-mediated gene transfer into COS-7 cells was substantially increased by chloroquine Luciferase

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activity was enhanced  15-fold and 55-fold for

com-plexes containing 43 and 64.5 lg HMGB2186,

respect-ively Taken together, these data show that HMGB2186

on its own is able to mediate nonviral gene delivery,

and strongly suggest that HMGB2186–DNA complexes

enter the cells through the endocytic pathway

Construction of HMGB2186derivatives containing the TAT PTD or the SV40 T-antigen NLS

To investigate whether HMGB2186-mediated gene transfer can be improved by including in the molecule

a cell-penetrating peptide, the PTD of the HIV-1 TAT

A

B

Fig 2 Functional characterization of purified HMGB2186 (A) DNA binding was analyzed by agarose gel electrophoresis of 0.5 lg pCMS-eGFP-E2C-Luc plasmid DNA in the absence of protein (lane 1), or after incubation with the indicated amounts of recombinant HMGB2 186

(lanes 2–5) The positions of supercoiled and open circular DNA, and protein–DNA complexes are indicated by arrows (B) Binding of HMGB2186to the surface of HeLa cells (left panel) and COS-7 cells (middle panel) was investigated by FACS analysis Cells were incubated with the indicated concentrations of purified HMGB2 186 protein Then bound protein was detected with Myc-tag-specific antibody 9E10 fol-lowed by fluorescein isothiocyanate-conjugated (HeLa) or phycoerythrin-conjugated (COS-7) anti-mouse IgG Control cells were incubated with antibodies in the absence of HMGB2186(open area) Mean fluorescence values (arbitrary units) were calculated from the COS-7 FACS experiments and plotted against the protein concentrations used (16.5 n M to 18.59 l M ) (right panel) HMGB2 186 -mediated gene transfer into COS-7 cells in the absence (C) or presence of 100 l M chloroquine (D) Cells were seeded at a density of 7 · 10 4

cells per well 24 h before transfection Transfection complexes were formed by incubating the indicated amounts of purified HMGB2186with pCMS-eGFP-E2C-Luc reporter plasmid before addition to the cells in normal growth medium (2.3 lg DNA per well) Control cells were treated with poly( L -lysine) (pL)–DNA complexes (open bar) After 4 h the medium was exchanged and cells were grown for another 40 h before they were harvested for analysis Luciferase activity is expressed in relative light units (RLU)Æ(mg total protein))1.

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protein (amino acids 47–57) flanked by additional

gly-cine residues was fused to the N-terminus of the

HMGB2186 fragment (Fig 3A; TATPTD sequence

shown in Table 1) This TAT fragment also includes a

nonclassical NLS [29] Therefore, to examine the

pos-sible effect of a heterologous NLS on HMGB2186

-mediated gene transfer independent of cell-penetrating

activity, a similar HMGB2186 derivative was

construc-ted which carries the classical NLS of the SV40 large

T-antigen [30] at the N-terminus (Fig 3A; SV40NLS sequence shown in Table 1) TATPTD-HMGB2186 and SV40NLS-HMGB2186proteins were expressed in E coli and purified from bacterial lysates as described above for unmodified HMGB2186 As expected, in compari-son with HMGB2186, a slight increase in the apparent molecular mass was found for the fusion proteins in SDS⁄ PAGE and immunoblot analysis with antibody against HMGB2 (Fig 3B)

A

B

C

Fig 3 (A, B) Bacterial expression of HMGB2186derivatives carrying the TAT PTD (TATPTD; amino acids 47–57) or the NLS of SV40 large T-antigen (SV40NLS) (A) Schematic representation of the TATPTD-HMGB2186and SV40NLS-HMGB2186expression cassettes also encoding C-terminal Myc (M) and polyhistidine (H) tags, inserted into plasmid pSW5 (B) SDS ⁄ PAGE (lanes 1, 2) and immunoblot analysis (lanes 3–5)

of purified SV40NLS-HMGB2186(lanes 1, 5) and TATPTD-HMGB2186(lanes 2, 4) in comparison with unmodified HMGB2186(lane 3) The pro-teins were identified with an HMGB2-specific antibody followed by horseradish peroxidase-coupled secondary antibody and chemilumines-cent detection (C) DNA binding was analyzed by agarose gel electrophoresis of 0.5 lg pCMS-eGFP-E2C-Luc plasmid DNA in the absence of protein (lanes 1, 6), or after incubation with the indicated amounts of recombinant SV40 NLS -HMGB2 186 (lanes 2–5) or TAT PTD -HMGB2 186

(lanes 7–10) The positions of supercoiled and open circular DNA, and protein–DNA complexes are indicated by arrows.

Table 1 N-terminal amino acid sequence and calculated isoelectric point of HMGB2 derivatives.

IBB-HMGB2186 MPRHHHHHH-AARLHRFKNKGKDSTEMRRRRIEVNVELRKAKKDDQMLKRRNVSSFPD-GT-GKGD 9.99

a Sequences of functional peptide domains are underlined Positively charged amino acids are indicated in bold The first four residues of the HMGB2 1–186 fragment are shown in italics The N-terminal Met residue, His-tag and sequences encoded by cloning linkers are also inclu-ded b Isoelectric points were calculated using Expasy (http://www.expasy.org/cgi-bin/protparam).

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The DNA-binding activity of purified TATPTD

-HMGB2186 and SV40NLS-HMGB2186 proteins was

analyzed in gel retardation experiments as described

above As shown in Fig 3C, in the presence of 1.7 or

1.8 lg of the proteins, 0.5 lg pCMS-eGFP-E2C-Luc

plasmid DNA was markedly retarded in the agarose

gels, indicating effective DNA binding and complex

formation

TATPTD-HMGB2186and SV40NLS-HMGB2186

mediate gene transfer

To examine the gene-transfer activity of HMGB2186

fusion proteins, protein–DNA complexes were

pre-pared by mixing increasing amounts of HMGB2186,

TATPTD-HMGB2186 and SV40NLS-HMGB2186 with pCMS-eGFP-E2C-Luc DNA (2.3 lg per well) as des-cribed above Transfection complexes were added to COS-7 and human HepG2 cells in complete growth medium containing serum for 4 h Luciferase activities were determined 40 h later In both, COS-7 and HepG2 cells, gene delivery mediated by TATPTD -HMGB2186 and SV40NLS-HMGB2186 was more efficient than HMGB2186-mediated transfection (Fig 4A,D) Maximal luciferase activity in COS-7 cells was achieved using 16.5 lg TATPTD-HMGB2186

(molar protein to DNA ratio of 1270 : 1), which was

38 times higher than after HMGB2186-mediated transfection with 13 lg of the unmodified protein (molar protein to DNA ratio of 1070 : 1), and still

A

-HMGB2 186 and TAT PTD -HMGB2 186 COS-7 (A, B), HeLa (C) or HepG2 cells (D, E) were transfected with protein–DNA complexes containing 2.3 lg pCMS-eGFP-E2C-Luc reporter plasmid and the indicated amounts

of purified SV40NLS-HMGB2186or TATPTD -HMGB2 186 proteins in the absence (A, D) or presence of 100 l M chloroquine (B, C, E) as described in the legend of Fig 2 Protein– DNA complexes prepared with unmodified HMGB2 186 were included for comparison Luciferase activity is expressed in relative light units (RLU)Æ(mg total protein))1.

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seven times higher than with 52 lg HMGB2186 (molar

protein to DNA ratio of 4200 : 1; Fig 4A, left and

right panels) In HepG2 cells, TATPTD-HMGB2186

was more than three times more effective than

HMGB2186 at the highest protein amounts used

(Fig 4D) Unexpectedly, luciferase activities measured

after SV40NLS-HMGB2186-mediated gene delivery into

COS-7 and HepG2 cells were very similar to those

obtained after TATPTD-HMGB2186-mediated

transfec-tion at comparable molar protein to DNA ratios For

gene delivery into HepG2 cells, SV40NLS-HMGB2186

was even slightly more effective than TATPTD

-HMGB2186(Fig 4A,D, middle panels)

As inclusion of the TATPTD domain did not

enhance transfection efficiency more than inclusion of

the SV40NLSdomain, the NLS function of TAT rather

than its membrane-translocating properties may be

responsible for the enhanced reporter gene expression

observed in comparison with HMGB2186 Therefore,

to analyze the possible involvement of the endocytic

pathway during TATPTD-HMGB2186-mediated and

SV40NLS-HMGB2186-mediated gene transfer, the effect

of chloroquine on transfection efficiency was

investi-gated, with HeLa cells included in the analysis in

addition to COS-7 and HepG2 cells As shown in

Fig 4B,C,E, in all three cell lines not only HMGB2186

-mediated and SV40NLS-HMGB2186-mediated, but

also TATPTD-HMGB2186-mediated gene delivery was

enhanced by chloroquine to a similar degree in

com-parison with transfection by the respective proteins in

the absence of an endosomolytic reagent These results

suggest that TATPTD-HMGB2186 protein–DNA

com-plexes may indeed enter cells primarily via an

endo-somal pathway, rather than by direct membrane

translocation as originally hypothesized for TATPTD

-containing fusion proteins

An HMGB2186derivative carrying the IBB of

importin-a displays enhanced gene-delivery

activity

The viral TATPTD domain can function as a

nonclassi-cal NLS by direct interaction with importin-b [29] To

investigate whether attachment of an endogenous

cellu-lar importin-b binding sequence to HMGB2186

enhan-ces its gene-delivery activity to a similar extent, the

IBB of human importin-a2 (amino acids 11–58)

together with an N-terminal His-tag was fused to the

HMGB2186sequence (Fig 5A; IBB sequence shown in

Table 1) The resulting IBB-HMGB2186 fusion protein

was expressed in E coli as described above for

HMGB2186 After purification, IBB-HMGB2186 could

be identified as the major band on SDS⁄ PAGE and

immunoblot analysis, and DNA-binding activity sim-ilar to that of HMGB2186was confirmed in a gel retar-dation assay

The gene-transfer activity of IBB-HMGB2186 was investigated in transfection experiments as described above using COS-7 cells HMGB2186, SV40NLS -HMGB2186 and TATPTD-HMGB2186 containing com-plexes were included for comparison As controls, gene-transfer complexes were also prepared with poly(l-lysine) and polyethyleneimine (PEI) Surpris-ingly, in the absence of chloroquine, gene transfer mediated by IBB-HMGB2186 was clearly less efficient than SV40NLS-HMGB2186-mediated and TATPTD -HMGB2186-mediated transfection at similar protein to DNA ratios, and was comparable to gene delivery mediated by unmodified HMGB2186 (Fig 5B) In stri-king contrast, in the presence of chloroquine, IBB-HMGB2186-containing complexes were remarkably effective, with ensuing luciferase activities higher than those achieved after transfection with TATPTD -HMGB2186–DNA complexes (Fig 5C) Importantly, with the exception of HMGB2186, which in this experi-ment was used at suboptimal protein concentrations, gene transfer mediated by the recombinant HMGB2186 derivatives was comparable to or more efficient than poly(l-lysine)-mediated transfection Not unexpectedly, transfection of cells with PEI, which is considered to

be one of the most efficient nonviral gene-delivery agents currently available, was still more effective than IBB-HMGB2186-mediated gene transfer in the presence

of chloroquine However, the differences were not dramatic, with luciferase activities measured after IBB-HMGB2186-mediated and PEI-mediated transfec-tion being of the same order of magnitude (less than fourfold difference; Fig 5C)

To analyze whether IBB-HMGB2186-mediated gene delivery is dependent on specific cell binding similar to that found for uncomplexed HMGB2186, competition experiments were performed COS-7 cells were pre-treated for 15 min with increasing amounts of IBB-HMGB2186 or unmodified HMGB2186 protein before IBB-HMGB2186–DNA complexes at an optimal pro-tein to DNA mass ratio of 8.2 were added Control cells were treated with IBB-HMGB2186–DNA com-plexes in the absence of competitor As shown in Fig 6, in the presence of an amount of free IBB-HMGB2186 comparable to the amount of protein in the complex, transfection efficiency was only 37% of controls, and was reduced further to 22% if the con-centration of free IBB-HMGB2186 was doubled Free unmodified HMGB2186 also affected transfection effi-ciency of IBB-HMGB2186–DNA complexes, but to a lesser extent than identical molar concentrations of

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free IBB-HMGB2186 (reduction to 66% and 43% of

controls) These data suggest that IBB-HMGB2186–

DNA complexes bind to the cell surface primarily via

the HMGB2186 domain and to the same structures

recognized by uncomplexed HMGB2186derivatives

The pCMS-eGFP-E2C-Luc reporter plasmid in

addition to luciferase also encodes eGFP, which allows

identification of transfected cells individually In a

separate experiment, COS-7 cells were incubated in the

presence of chloroquine with protein–DNA complexes

at a molar protein to DNA ratio of  1200 : 1 as

des-cribed above At 20 h after transfection, cells were first

analyzed by fluorescence microscopy (Fig 7A),

fol-lowed another 20 h later by FACS analysis for

quanti-fication of eGFP-expressing cells (Fig 7B) Confirming

the results obtained in the luciferase assays, in the

presence of chloroquine, IBB-HMGB2186was again the most effective HMGB2186 derivative resulting in suc-cessful transfection and measurable eGFP expression

in 13% of the cells, which compares well with PEI-mediated transfection (19% of eGFP-positive cells) Taken together, these data suggest that IBB has no effect during uptake of protein–DNA complexes via the endocytic pathway, but upon release from endo-somes with the help of chloroquine may serve as a pure NLS, greatly improving transport of plasmid DNA to the nucleus and enabling efficient gene expres-sion In contrast, SV40NLSand TATPTD may also con-tribute other activities that improve nonviral gene delivery, as indicated by their ability to enhance trans-fection efficiency already in the absence of an endo-somolytic reagent

A

B

C

Fig 5 (A) Bacterial expression of an HMGB2 186 derivative containing IBB (amino acids 11–58) of human importin-a2 The IBB-HMGB2186expression cassette also encodes a C-terminal Myc (M), and N-ter-minal and C-terN-ter-minal polyhistidine (H) tags, inserted into plasmid pSW5 Shown below are SDS ⁄ PAGE (lane 1) and immunoblot analysis (lane 3) of purified IBB-HMGB2186

in comparison with unmodified HMGB2186 (lanes 2, 4) The proteins were identified with an HMGB2-specific antibody followed

by horseradish peroxidase-coupled secon-dary antibody and chemiluminescent detec-tion DNA binding was analyzed by agarose gel electrophoresis of 0.5 lg pCMS-eGFP-E2C-Luc plasmid DNA in the absence of protein (lane 1), or after incubation with the indicated amounts of recombinant IBB-HMGB2186(lanes 2, 3) The positions of supercoiled and open circular DNA, and protein–DNA complexes are indicated by arrows (B, C) IBB-HMGB2186-mediated gene transfer COS-7 cells were transfected with protein–DNA complexes containing 2.3 lg pCMS-eGFP-E2C-Luc reporter plas-mid and the indicated amounts of purified IBB-HMGB2 186 , or HMGB2 186 , SV40 NLS -HMGB2186, or TATPTD-HMGB2186proteins for comparison in the absence (B) or pres-ence of 100 l M chloroquine (C) as described

in the legend of Fig 2 Control cells were treated with poly( L -lysine) (pL)–DNA com-plexes, or PEI–DNA complexes at an N ⁄ P ratio of 10 (open bars) Luciferase activity is expressed in relative light units (RLU)Æ(mg total protein))1.

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The ability to condense DNA is essential for a nonviral

vector to be successful as a gene-delivery reagent [4]

Although synthetic vectors are most commonly used

for nonviral gene transfer, certain DNA-condensing

proteins of mammalian origin have also been shown to

facilitate cellular uptake of plasmid DNA Previous

studies on histones and HMG proteins as gene-delivery

reagents mainly used full-length proteins purified or

enriched from animal tissues [5–11], whereas only a few

groups have so far attempted to utilize such proteins in

recombinant form [12,14] Here we have generated a

novel recombinant derivative of the human HMG

pro-tein HMGB2, which facilitates nonviral delivery of

plasmid DNA into tumor cells By complementing

the DNA-binding activity of this HMGB2186 variant

with additional functional domains from heterologous

proteins, we achieved a marked increase in

protein-mediated transfection

HMGB2 is a member of the HMGB subfamily of

nonhistone chromatin proteins, which also includes

HMGB1 and the more recently discovered HMGB3

[31,32] HMGB proteins have little or no sequence

spe-cificity and bind preferentially to certain (distorted)

DNA structures [32,33] Thereby the acidic C-terminus

appears to control DNA binding, as truncated

HMGB1 and HMGB2 lacking this sequence displayed

increased affinity for DNA [23,34–37] Deletion of the acidic tail also largely abolished the differences in DNA binding between the three HMGB proteins [23] Consequently, as a reagent for nonviral gene delivery,

we constructed a truncated HMGB2 derivative that encompasses amino acids 1–186 of the human protein, but lacks the acidic C-terminal part Whereas in a previous report bacterial expression of full-length HMGB1 had only resulted in very low amounts of recombinant protein [38], here we encountered no problems with regard to expression of truncated HMGB2186 in E coli, and high yields of soluble recombinant protein could be obtained after purifica-tion from bacterial lysates under native condipurifica-tions [up to 4 mgÆ(L culture))1]

Purified HMGB2186 was able to condense plasmid DNA in a concentration-dependent manner, indicated

by marked retardation of the resulting protein–DNA complexes in an agarose gel Starting at a molar pro-tein to DNA ratio of 1050 : 1 (representing an HMGB2186 protein to DNA mass ratio of 5.6), maxi-mum retardation of plasmid DNA was achieved Pre-viously for recombinant full-length HMGB1 expressed

in yeast, in a similar assay, a protein to DNA ratio of

7000 : 1 was required [12] This suggests that removal

of the acidic tail indeed facilitated enhanced DNA binding of the protein, even if general differences between HMGB1 and HMGB2 may have partially contributed to this effect As shown by FACS analysis, HMGB2186 also bound to the surface of established tumor cell lines in a concentration-dependent and satu-rable manner Although at present the exact nature of this interaction remains unclear, our data suggest spe-cific binding of HMGB2186to defined target molecules rather than unspecific attachment to the cell mem-brane This also appears to be the case for HMGB2186 derivatives complexed with DNA, as transfection efficiency of preformed IBB-HMGB2186–DNA com-plexes was significantly reduced when free HMGB2186

or IBB-HMGB2186 proteins were added as competi-tors Likewise, gene transfer was decreased when HMGB2186 derivatives were present in too high amounts in transfection complexes For HMGB2, in contrast with the related HMGB1 molecule, so far no extracellular activity has been reported [32,39] Never-theless, owing to the high homology between these proteins (80% amino-acid sequence identity), HMGB2 may bind to the same or similar cell surface molecules

as HMGB1, which include the receptor for advanced glycation end products (RAGE) [40] and syndecan-1 [41] Interestingly, PEI–DNA complexes have also recently been found to be internalized by adherent cells after binding to syndecans [42]

Fig 6 Effect of uncomplexed HMGB2186derivatives on

transfec-tion efficiency of IBB-HMGB2 186 –DNA complexes COS-7 cells

were transfected in the presence of 100 l M chloroquine with

protein–DNA complexes containing 2.3 lg pCMS-eGFP-E2C-Luc

reporter plasmid and 18.8 lg purified IBB-HMGB2 186 protein

(protein ⁄ DNA mass ratio of 8.2) as described in the legend of

Fig 2 Before transfection, cells were treated for 15 min with

uncomplexed IBB-HMGB2 186 or HMGB2 186 proteins as indicated.

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In in vitro transfection experiments, treatment of

dif-ferent tumor cell lines with HMGB2186–DNA

com-plexes resulted in transient expression of luciferase

and eGFP reporter genes Depending on the protein

amounts used, gene transfer was more efficient than

with poly(l-lysine)–DNA complexes, and was not

inhib-ited by the serum in the culture medium Although in

these experiments poly(l-lysine) was used at amounts

favoring the formation of electroneutral complexes, and

no attempt was made to optimize transfection by this control reagent, gene delivery by modified HMGB2186 derivatives compared well with PEI-mediated transfec-tion at optimal N⁄ P ratios previously shown to be far superior to poly(l-lysine) [43] At the concentrations tested, cell viability was not affected by protein–DNA complexes containing HMGB2186 or HMGB2186 fusion proteins (data not shown) Addition of the endo-somolytic reagent, chloroquine, strongly enhanced the

A

B

Fig 7 Analysis of eGFP expression after transfection with protein–DNA complexes containing HMGB2186derivatives COS-7 cells were transfected with protein–DNA complexes containing 2.3 lg pCMS-eGFP-E2C-Luc reporter plasmid and the indicated amounts of purified HMGB2 186 , SV40 NLS -HMGB2 186 , TAT PTD -HMGB2 186 , or IBB-HMGB2 186 proteins in the presence of 100 l M chloroquine as described in the legend of Fig 2 Control cells were treated with poly( L -lysine) (pL)–DNA complexes, or PEI–DNA complexes at an N ⁄ P ratio of 12 (A) Micro-scopic analysis of eGFP expressing cells 20 h after transfection Corresponding representative fields after fluorescence and bright field micro-scopy are shown (B) Quantification of eGFP-expressing cells by FACS analysis At 40 h after transfection, cells were collected and analyzed

by flow cytometry Untreated COS-7 cells were used as a control The cut-off for eGFP expression was set at the fluorescence intensity at which 99.84% of the control cells displayed a lower fluorescent signal The bars represent the percentage of eGFP expressing cells (1 · 10 4

cells per well analyzed in duplicate) Magnification, 100·.

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